Great OPs:
Soul Eater
Soul eater's opening is just so impressive. The animation is MIND BLOWING with all the perspective changes and general excellence in animation. The song paces it all very well.
Fate Zero
Holy **** how to do a shounen opening 101. This opening used to and still does always give me goosebumps. The only complaints I'd have is lack of cool animation and the burst of activity is somewhere around the middle (which does allow for buildup).
zetsuen no tempest
Zetsuen no tempest did the smart thing and used anime scenes for its opening, giving it great animation. A bit of a generic yet cool song. All around pretty good.
serial experiments lain
SEL did great with its song. Imagery is very well done and fits the theme of the show as well as some perspective magic (which was really hard to pull off especially the day and age this was made)
tokyo ravens
TR's opening is a perfect mix of mystery and cool. That's basically all there is to it.
samurai champloo
Cool song that actually made my playlist, with excellent animation (that I'm pretty sure gets used in the show too but whatever)
Great songs:
Cowboy Bebop movie (ask DNA)
natsume yuujinchou (ano hi time machine)
chihayafuru (youthful)
mushishi 1 and 2 (sore feet song & shiver)
psycho pass (abnormalize)
hellsing (logos naki world)
JoJos part 2 (bloody storm)
tasogare otome x amnesia
Shoutout for using a full metal song in an anime OP about a girl
as for EDs, I don't check EDs often but one that comes to mind is Space Dandy's ED