Nolans TDK trilogy takes the cake for me. You've got a fantastic origin story in Batman Begins, which pulled Batman out of the darkness after Batman and Robin. Batman Begins fleshed everything out, took it's time and provided us with a fantastic introduction to Bruce Wayne, Batman, and his world. Memorable villains like Ras Al Ghul and Scarecrow played by some of the industries best.
Then you have The Dark Knight, which builds upon and expands Bales Batman while giving us an absolute rollercoaster of a film with post 9/11 themes of terrorism, and how far people can be pushed without losing their humanity. Obviously, the elephant in the room is Ledgers iconic portrayal of the Joker which has gone down as not just the greatest villain portrayal in comic book movies, but one of the greatest in cinema standing along side Darth Vader and the like. The Dark Knight redefined and transcended the comic book movie genre. It's accolades speak for themselves.
The Dark Knight rises ties everything set up in Batman Begins and has it come full circle. Bruce began his journey in Batman Begins falling down a well trapped with his greatest fear. He literally gets broken in TDKR and climbs out to save the city he helped protect and inspire. Along with Tom Hardys memorable iteration of Bane, we have a movie that is emotional, epic, and serves as a definitive ending to a fantastic trilogy. People like to pick this movie apart for things such as the action and such, but that sewer fight and the emotional drive behind it is so damn effective.
I LOVE the Raimi trilogy and particularly the first 2 films defined and introduced my love for those kinds of movies. both films are in my top 5 comic book movies ever, with Spider-Man 2 coming in at #2 behind The Dark Knight. The Dark Knight and Spider-Man 2 are the gold standard of the genre. Spider-Man 3 is a flawed movie, but i still enjoy it for what it is. I'll always hold that trilogy close to my heart, and it's still, far and away, the best live action adaption of the charatcer. I also think the first 2 Raimi films are better than every Marvel film since. Yeah I said it! but for me, the Nolan trilogy edges it out overall.