I never saw 'Angel' when it was on real time, I actually didn't start watching until this summer when I borrowed my friend's Season 1 DVDs for like a month and watched them a million times. The first few episodes I wanted Cordelia and Doyle together but my favorite C/A moments are in Room w/ a Vu.
He brings her the dorky cactus, which I just thought was new for Angel and his social skills.
Angel is the one that is all touchy/feely when dragging her from the apartment and telling her she's "better than that". And his whole forceful, "You're Cordelia Chase..." blah blah blah, which to me means that Angel knows more about her than she was the head of the Cordettes and cared a lot about shoes. From then on I was all about C/A.
Parting Gifts is another one of my favorite episodes for C/A. Especially when he saves her and she hugs him while still in game face. She's accepted that part of him and isn't afraid of it.
Most of my moments come from Season 1, just because I have them memorized more.
Anyways, that was a bit of babbling but it's late. Thought I'd add my two cents.