I tried to go in order for seasons of specific moments, 12 songs to cover so many seasons is not easy 😛
Buffy:
Smells Like Teen Spirit-Nirvana (s1)
Working Class Hero-Greenday (Ending of s1)
While Your Lips Are Still Red-Nightwish (Bangel, s2/Passion)
We Will Rock You-Queen (Ending of s3)
Everything Will Be Alright-The Killers (s5, maybe when Buffy finds out about Dawn)
Let It Be-The Beatles (The Gift)
Comfortably Numb-Pink Floyd (beginning of s6)
Famous Last Words-My Chemical Romance (s6)
Kryptonite-3 Doors Down (s6, Normal Again)
End of All Hope-Nightwish (s7)
Born To Die-Lana Del Rey (this one just fits on so many places, I can't decide where it would fit best)
Army of Me-Bjork (comics)
For Angel:
Fallen Angel-Sirenia (opening)
Lonely Day-System of a Down (s1, After Doyle's death)
Somebody That I Used to Know-Gotye (s2, it's suppose to be a love song, but I like it for the group as they break apart and Angel goes all dark)
Every Breath You Take-The Police (Angel to baby Connor)
The Unforgiven-Metallica (Angel tried to kill Wes, s3/Wes s4)
End of Me-Apocalyptica (as they are lowering Angel under the sea, any Apocalyptica song is super for Angel though)
Wild World-Cat Stevens (I kinda like this one for Cordy, or surrounding Cordy's death, which was the most missed opportunity on the show, happy-ish song for a character that deserved better)
Still Worth Fighting For-My Darkest Days (s5, Fred dies)
High Hopes-Pink Floyd (Not Fade Away)
End of Everything-Tarot (After the Fall)
Angels Fall First-Nightwish-(closing)