This is a cool idea and I hope more members here post their thoughts!
Here are mine.
Series: It is VERY hard for me to choose here. I think BtVS is a lot more funny and campy. Angel is darker and more mature at times. My favorite usually depends on my mood of the moment. Right now i'd say BtVS. But again i'd probably say they're equal for me if someone randomly asked me.
Seasons: BtVS is S5, Angel is S4. For Buffy it's again CLOSE, I like s2 and 3 a lot too but s5 usually win out because it has more realistic drama to me, and also I really liked Buffy/SMG in that season. Also the last season where Giles was awesome =/
As for Angel, I know it isn't a popular choice here. I know why peoples don't like it. But as for me, when I watched that season I was SO freaking hooked I got so much into it. No other seasons in the series had that effect on me. I think it's mostly because of the main arc(up until Jasmine, it was less fun once there for me), and there was so many shocking moments for me through those first fifteens/sixteens episodes. As an example... I always complained about how I hated the fact there was so many peoples in BtVS in s7, too many boring and useless characters. Well in Angel S4, at the point where the Beast is out, Lilah get into it, you got Gavin(which I expected to be a bigger player in the end), Faith, Angelus and the whole group with Gwen, it's awesome! There's a bunch of characters but they actually work with the story and ain't just there for background. I have so much to say about that season... First episode is AWESOME and then the premise with Cordy coming back, the hilarious 'Spin the bottle' episode, and then you got that spooky and also unexpected episode where W&H get destroyed. The Beast, then guessing who is behind all this(sadly it wasn't as great a reveal as it could have been). Then right in the mix of all that stuff, you bring Angelus back and you got neat confrontations between each character and him. Followed by Faith coming back and actually being the 'hero' somewhat =P I just loved that season. I'll save some parts for the 'best moments' down there though lol!
Episodes: This is tricky, because you wanna pick one episode that stand out by itself, not a bigger arc like what I was mentioning up there. It's between 'You're Welcome' and 'Smile Time' for Angel. Actually as stand out episodes go in Angel, they are mostly in s5 for me =P Smile Time win it for me in the end just because Angel as a puppet is hilariously good, his frown and then vampire puppet!!!! HAHAHAHA!
As for BtVS, Band Candy is really up there. Everyone is hilarious in that episode, and you got Ethan! It's just an episode i'll never get tired of. Total comedy. Obviously Hush was really good too, and all the others well known episodes like OMWF, The Gift and such. Oh and I can't forget Restless, that was amazing and I watched it countless times to decipher every scene meaning. But since I got to make a choice, i'll pick Band Candy, it's just such good fun!
Moments: Now there's a lot!
Angel
- Spike narrating the whole scene in 'In The Dark' after Angel saved a girl, 'To the Angelmobile, away!' hahahaha.
- Buffy crying and looking so desesperate in IWRY when there is less than a minute left =( That was sad.
- Faith going crazy on Angel at the end of 'Five by Five' and asking him to kill her. That whole scene with Wes dropping the knife at the end while the rain kept pouring was really something.
- When Angel finally get mad and snap at Kate after both his friends got really hurt and she started bitching at him again. Oh my god, I was like, ABOUT TIME!
- Angel firing his friends =(
- When Wes come tell him that even if he stopped, they will keep up the good fight, and Angel stay silent and then tell himself 'let them do the good fight, someone has to do the war'.
- Lindsey whole scene in W&H room when he talk about his 'new hand' and how he doesn't control it. That was both hilarious and great. Because he actually saved Lilah right there.
- Cordy yelling like crazy when Lorne's head start talking(after being cut), HAHAHAHAHA! That was awesome =P
- The whole taken hostage scene at Caritas with Gunn's old crew. I always liked that part! Go Fred!
- Scene in 'Billy' when Fred come to see Wes after what happened and he start crying after she goes.
- Darla staking herself to give birth to Connor... another scene in the rain. I love those.
- In 'Couplet', when Angel compare his height to Groo, hahahah! That's why you like Angel!
- When Wes plan on taking Connor and Lorne appear and he read him. That scene make me feel bad for both =x Wes 'betraying' is sad but understandable.
- ****Most likely biggest shocking moment for me in Angel**** Angel coming to see Wes at the hospital, acting alright with his friends and talking nicely to Wes until he just suddently try to smother him and goes totally crazy.
- When that huge demon comes out of the gate in 'The Prize' and then Connor appear and kill it in one hit just before saying 'Hi Dad'! Always give me chills.
- Last scene in 'Tomorrow' with Cordy going up and Angel down.
- Shocking moment for me was when Fred come up with food for Connor in 'Deep Down' and then just suddently(kinda like Angel with Wes previously) tell him she hope he suffers and use a stun gun on him.
- Also the scene when Angel has a daddy-son talk with Connor right after is pretty good.
- Wes karate chops, Angel touching his throat after he realize he doesn't have an accent(LOL!) and Angel reaction when he see he has no reflection in 'Spin the Bottle'.
- Fight scene with the Beast on top of that building, Wes is bad ass there =P
- Opening scene of Long Day's Journey with Gwen and that guy who just get killed suddently by the Beast. That was a shock.
- Realizing Angel was just dreaming about the whole story in 'Awakening' and then hearing Angelus laugh(great!). I sure didn't see that coming the first time.
- 'Evil' Cordy killing Lilah with the knife... that was another freaking shocker for me.
- Lorne's 'magic eight ball'. Cordelia has been a bad girl! Hahaha.
- Fred walking alone with that eery music and everyone kneeling to Jasmine at the end of 'Shiny Happy People'.
- Even though I knew that one(sadly!), Spike coming out of the amulet and the reaction of everyone, awesome!
- Wes killing his 'Father' without ANY hesitations... that was a huge shock right up there for me.
- The scene with the phone at the end of 'You're Welcome' when Angel find out Cordy never woke up(and is dead) =( Saddest moment for me.
- Puppet Angel with his sword walking out of his office with Wes and Fred behind, lmao!
- Puppet Angel turns into Vampire Puppet Angel!
- Fred painful death in the arms of Wes =( That was awesome acting on both sides.
- Kick ass scene in 'Time Bomb' where Illyria kill the whole group in a few seconds... love how Angel turn to dust while flying, lol.
- When Angel reveal his plan to his friends and they all lift their hands.
- Last look between Wes and Angel.
- 'Do you want me to lie to you now?'
- And obviously the alley scene where Gunn says 'You take the 30,000 on the left...' and Angel close it with my favorite quote 'Let's go to work!'.
Buffy(i'm gonna cut down on the number of moments here, lol =P)
- Xander yellow crayon speech to Willow at the end of s6.
- Buffy running to catch Riley in time.
- Final scene in the Gift with everyone staring at Buffy's corpse.
- Buffy killing Angel and the whole part after =(
- Buffy's 'Mommy' at the start of 'The Body'.
- The scene from my sig.
- Whole scene in Earshot in the library when they find out Buffy can read minds.
- Scene in Band Candy with Buffy interrogating Ethan and Giles cheering her on to hit him, haha!
- Buffy smashing the Master's bones in 'When she was bad'.
- Giles finding the note left by Ethan at the end of 'The Dark Age'.
- Angel yelling Buffy's name after they slept together in Surprise and that he's about to lose his soul in that alley.
- Rocket launcher, need I say more?!
- Argue between Buff and Xander in 'Dead Man's Party'.
- Angel appearing at the end of 'Faith, Hope and Trick'.
- Scene at the end of 'Amends' when Angel and Buffy talk before the sun comes up.
- Xander not telling anyone anything at the end of 'The Zeppo'.
- 'Best Actor' 'No, second best' moment in 'Enemies'.
- Scene in the school with the Mayor and everyone in 'Choices'.
- Dream sequence in 'Graduation Part II'.
- Everyone standing up for Tara in 'Family'.
- Pissed off Willow in 'Tough Love' when she tells Glory 'I owe you pain!'.
- Showdown between Giles and Willow in 'Grave'.
- Dawn scene in 'Conversations with Dead People' when she keeps yelling to that thing to get out of the house, LOL! Go Dawn.
- When you see what Buffy saw(the huge army of Uber Vamps).
- Scene between Buffy and Spike in 'Touched' when she ask him to stay.
- Spike snapping at everyone for kicking Buffy out of her house.