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20.Corbin Fries (Conviction)
Sleazy and willing to use/kill his own child to get what he wants. A truly despicable person, but also a very memorable character.
19. Magnus Hainsley (Just Rewards)
Not much depth to this character, but I did like that his motive was money, so rarely do we see this any more as it's become something of a cliche in recent years. Of course, he's also memorable as the guy that Spike took over to fight Angel.
18. Agent Hauser (Conviction)
Evil through and through, Hauser is a fairly interesting one-off character. His final speech to Angel, I think, says it all. "I believe in evil."
17. Roger Wyndam-Pryce/Cyborg (Lineage)
The fact that he completely fooled Wesley tells us just how correctly he 'portrayed' the real Roger and that makes for a very interesting character study (though mostly of Wesley, of course). The final plot twist reveal also leaves this very memorable.
16. Prince of Lies (Why We Fight)
Well, he's just fun, isn't he?
15. Marissa (Deep Down)
I don't know why she sticks out to me, but she does. In a very short amount of time, she manages (along with the writers) to make herself into a very three-dimensional vampire with a backstory and a personality. I quite enjoyed that.
14. Maude Pearson (Rm w/a Vu)
"Oh, come on. If anyone really cared about you, would you be here? People let you end up here because they were happy to see you fail."
13. Denver (Reprise)
He's one of those fun one-off's that we don't need to see more of but is enjoyable on every re-watch.
12. Gwen, Files & Records (Dad)
Poor Lilah really needs to ask the right questions. That effect with her eyes was pretty cool, too.
11. Ilona Costa Bianchi (The Girl in Question)
Constantly spitting, boobs almost hanging out, thick Italian accent. She was a real character and I loved her!
10. Prima Ballerina (Waiting in the Wings)
Summer Glau. Need I say more?
9. Vocah (To Shanshu in L.A.)
Not only portrayed by an actor who plays another favorite one-off character of mine on SPN, but Vocah was a great last-minute villain for the finale. A spear-head of the law firm, if you will; the muscle. Very memorable, imo.
8. Penn (Somnambulist)
Jeremy Renner before the bow and arrow, he did a decent job of the character, both in flashbacks and present day. That the character was memorable long before I ever saw any MCU film says a lot.
7. Bethany Chaulk (Untouched)
Her power was very intriguing, her background awful and her entire thought process (offering herself to Angel) indicative of the kind of life she's led. Her connection with Lilah also helped make her story more interesting, to me.
6. Cindy Rabinowitz (Conviction)
Again, don't know why; she's pretty high for an appearance that lasted, maybe, 30 seconds. But listening to her singing There Once Was a Man, and seeing Lorne's face as he's listening...it's just very memorable and hilarious to me.
5. Numfar (Through the Looking Glass)
With or without the knowledge of who is behind the green makeup, this is just a great, funny performance. The kind of ridiculousness that AtS did very well, every now and then.
4. Rebecca Lowell (Eternity)
For a one-off character, she was in almost every scene, so it's hard not to put her on the list at all. She reaches this high spot for being a very complicated, real character, and not a caricature of some kind. She's still out there somewhere, aware of the supernatural but probably too self-involved to give it much thought.
3. Harriet 'Harry' Doyle (The Bachelor Party)
My only complaint is that we never saw her again. Her reappearance after Doyle's death could, potentially, have been pretty amazing. She could even have become a recurring guest character, what with her work with benign demons. But, even with just one episode, I still really enjoyed her, and her relationship with Doyle.
2. Dana (Damage)
The broken Slayer. The Council took her away, but I don't personally think there's any saving her. She'll be in a padded cell for the rest of her life, and that's just so depressing. The actress did a really good job with Dana and she's another one that I wanted more of.
1. Sam Lawson (Why We Fight)
He may be half the reason I love this underrated episode so much. His use in fan fiction is another reason he's here, I have to admit. His connection with both Angel and Spike, the fact that we don't really know if he's 'fully evil' or something different (thanks to being turned by a cursed-with-a-soul vampire), his desire to find a purpose even after being turned; I find his character endlessly fascinating and can't stop trying to figure him out. Thank God for fan fiction!
Dana (Damage) - I loved seeing the bad side to the spell in Chosen, showing how it was affecting girls who couldn't handle the power of being the Slayer. Dana was a great way to do this, and even though she doesn't get the most fleshed-out personality, I still found her a really interesting character.
Rebecca Lowell (Eternity) - I know this episode is a bit divisive, as is the character, but I found Rebecca very endearing and a somewhat tragic character, given the world she inhabited and the mental issues she was obviously dealing with, plus I liked her connection with Angel.
Harriet Doyle (Bachelor Party) - I liked getting to know more about Doyle's background and Harry was a very sweet and friendly character.
Matthias Pavayne/The Reaper (Hellbound) - a very unsettling and effective villain and I really like the actor who plays him (he also plays Death on Charmed, to great effect).
Penn (Somnambulist) - love seeing Jeremy Renner pre-Hollywood fame and he works well as this protegee of Angelus'. He's effectively creepy and very intriguing, and I like seeing more of Angelus' past, especially because we don't see a lot of vampires whom he sired.
Judy Kovacs (Are You Now Or Have You Ever Been) - Judy is a great character, she's interesting with a very sad backstory, she genuinely likes and connects with Angel but her paranoia and fear gets the better of her. I love that Angel sees her again as an old woman and gives her the forgiveness and peace she needs.
Tina (City Of) - Angel's first human connection in L.A., I found Tina very likable and sweet, and I felt quite sorry for her, as she was obviously longing for home and wishing she could escape her horrifying situation. I was very upset when she died.
Russell Winters (City Of) - He's a fun villain, even though he only turns up for a few scenes. You can see how he's charismatic and makes promises to these young, impressionable women, but how he's also very threatening.
Bethany Chaulk (Untouched) - I kind of hate the way her character is handled/treated within the narrative, but she's a very interesting character, especially given her powers and her horrific backstory. As @Puppet said, her connection to Lilah also makes her very interesting.
Alonna Gunn (War Zone) - I really wish we'd had more time with Alonna because she seemed like a great character; street-smart, sassy and doesn't take any of Gunn's crap. She was obviously resilient and a leader, like her brother. Would have loved to see more of her.
Vanessa Brewer (Blind Date) - she was such a creepy and effective villain. I loved that she was actually human, as so many of the bad guys are demons of vampires, it was interesting to see Angel actually take out a human character.
Numfar (Through The Looking Glass) - because he does the Dance of Joy!
Prima Ballerina (Waiting In The Wings) - Summer Glau does a lot with just a small amount of dialogue and I like her tragic backstory (referencing The Red Shoes).
Sunny (A New World) - Connor's first human connection other than Holtz, she was sweet to him and I liked their brief connection. Her death and Connor's reaction to it are very sad.
Magnus Hainsley (Just Rewards) - he's creepy but a lot of fun and I think the actor was having fun with the role, which is always good to see.
The Valet (The Trial) - I like the actor who played him and I liked that he was actually a truly neutral character, simply there to oversee the Trials but with no personal stakes in the outcome.
Barney (Parting Gifts) - I like how he comes across as affable and friendly but has a nastier side and I think the actor playing him did very well in switching between the two sides to his persona.
James (Heartthrob) - he was kinda pathetic, but I liked how he represented that obsessive, self-destructive love which seems to spring up in vampires often (makes me think of TVD or The Originals) and I liked the actor who played him.
Jheira (She) - I don't love the episode but Jheira is a very interesting character. I like how determined she was to save her people and how ruthless she was in this pursuit. Plus I liked the actress playing her and her makeup design was very cool.
The Demon Puppets (Smile Time) - somehow both hilarious and creepy at the same time, they were some of my favourite villains of Season 5.
There are people on this list who are not demons, nor vampires, but also not (fully) human. I kinda had to cheat a little to find 20 for the list
20. The Valet - Thank you to @RachM for reminding me of this character. I feel like we should've consulted each other before we made our lists, lol. 19. Thesulac - Truly a villain, he kept Judy with him for decades. His power, causing paranoia all around him, is also shown to be both terrible and hilarious. 18. Billy Blim - I'm one of the few who loves this underrated episode (Billy) and part of that is this guy, who is sufficiently creepy and a very successful villain. 17. Vocah - I had him on my other list. What can I say, he's played by Todd Stashwick, can't go wrong with him 16. Merl - A fun semi-guest on S2, his dynamic with Angel was always good for a laugh or two. 15. Barney - I just rewatched Parting Gifts yesterday and now feel I should've added him to my previous list. I'm honestly not sure how I could've forgotten him! 14. The Groosalug - He was around for too long, or he might've been higher, but I did enjoy his character; he was a truly good person, through and through. 13. Nina Ash - Only this low because she's technically human. Still, I'm counting her. My favorite of Angel's girlfriends, she was a character with so much potential. 12. Maude Pearson - Ghost counts, right? Oh, damn, I should've put Dennis on here, too, then... (he shares this spot with his mommy, kay?) 11. The Immortal - He was never even on screen but somehow he still became a character in his own right. I don't know, maybe I've read too much fanfiction 10. Marcus Hamilton - They totally made up for the boring Eve by giving us this great character (played by the equally great actor, Adam Baldwin). Loved his final fight scene with Angel in Not Fade Away so much. 9. Matthias Pavayne- A successfully creepy villain with a well-deserved (if frightening) final end. An eternity of solitude would certainly be my idea of Hell. 8. Sahjhan - He made S3 far more bearable and his dialogue around Holtz was always sharp and witty. 7. Skip - Of course he's here! Whether he was making Cordelia part demon (just wait), elevating her, or having his true identity discovered, he was always a great addition to any episode. 6. Jasmine - Once she was born (and played by Torres) that storyline suddenly got miles better. 5. Puppets - Once again, I'm embarrassed to have totally forgotten about them for the previous list, so here they get an extra special spot 4. Krevlornswath of the Deathwokclan - Lorney-Tunes!!! He was occasionally shafted, plot/character arc-wise, and I don't always agree with where they went with him, but damn if I don't love him anyway! 3. Cordelia Chase - Yes, I cheated! Technically she didn't become a (part) demon until S3, and we don't even know how big that part is, but dammit it still counts! She would probably have been no. 2 if they hadn't ruined her 2. Illyria - My beautiful smurf! 1. Allen Francis Doyle - Yeah, this was never any contest whatsoever. My sweet Doyle, I still miss him...
Mistres Meerna A New World
Ilona Costa Bianchi The Girl in Question
Alonna Gunn War Zone
Prima Ballerina Waiting in the Wings
Billy Blim Billy
Maude Rm w/a Vu
Virginia Guise will be Guise
Rebecca Lowell Eternity
Tamika Harms Way
Polo Smile Time
Trepkos The Ring
Roger Wyndam-Pryce/Cyborg Lineage
Judy Are You Now or Have You Ever Been?
Manjet Long Days Journey
Professor Seidel ( I love to hate him) Supersymmetry
Izzy - the red one in season 5?
The high priest demons from Pylea
Karaoke baby eating demon
demon from Birthday that the teen girl raised