Just picking one is difficult to do.
Bleach has a couple that I really enjoy. The season two opening by Uverworld, but I can't remember the name of the song. It was half about the animation and half about the song itself. But the whole thing really got me psyched up for the new episode of Bleach.
Also Season one ending one, for Bleach Life is like a Boat is a really good song. I think it came down a little about the imagery which was Rukia just very solemnly standing there in combination with the music.
Season two ending one (3rd ending total) Houki Boshi is one of my all time favorite songs period. It was really cool how they show off all of the squads one ending at a time, but also the song is really nice to listen to. I listened to it over 3000 times on my Windows Media Player before my laptop got reset. Just to give you an idea of how many times I've listen to it.
Most of the rest of Bleach's openings and endings have been pretty forgettable, I enjoy them yes, but the imagery itself is far better than the songs could hope to match. Though I will admit that Shojo S by Scandal has grown on me.
Every single Inuyasha song was perfect. I have all of the songs on my laptop that I listen to regularly. Sadly, since AS never showed the OPs past the first season I've never really seen the openings. So I only got to know the EDs and the songs. But I love all of the songs, Angelus, Every Heart, Brand New World, Itazurana Kiss, Fukai Mori, My Will, Every Little Thing, I am, Change the World, Come, Oawrinai Yume, One Day One Dream.
Outlaw Star's opening and ending I always watch whenever I watch the series. It remains the only series that I will always watch both OP and ED every single time. I love the song and animation, but the ED even more. I love the artwork that is in both EDs. The music that goes along with it is amazing too. Half of the reason that I watch the ED is simply because the artwork is so beautiful to behold. Though with how much I've watched it I've started singing along with it.
Fullmetal Alchemist fourth opening Rewrite by Asian Kung Fu Generation is always great to watch. You get to see a lot of the characters doing some crazy stuff that never happens in the series, but simply looks awesome as a battle.
Sakura Wars TV, the opening is really good, but the theme song that is the Sakura Wars theme song is so great to listen to. They use it for almost all of their games and anime I think. The style of song is so different and powerful that is such a thrill to listen to.
Gundam Wing Just Communication, Rhythm Emotion and Last Impressions, which were all the OP, plus Endless Waltz "theme song" are probably always going to be my favorite out of the Gundam series as a whole. Though Gundam 00 OPs are starting to sneak in there, which only seems right being similar to Gundam Wing in some ways.
Running down some others, Hitomi no Tsubasa from Code Geass 3rd OP. Kirari Takaramono from Love Hina Again, GITS:SAC and GITS:SAC 2nd GIG OPs, ex Dream from X TV, Kai no Mahou from Maburaho and Tomorrow from FMP, to name a few others.
I love OP/ED ^^
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