1. House of Five Leaves OP (immi, "Sign of Love") -- Fascinating music, with entrancing imagery that was also inexpensive to produce. Enjoyable both for itself and for how it sets up and gives pace to the show.
2. Shiki OP1 (Buck-Tick, "Kuchizuke") -- Dark vampiric modern rock, with outstanding images. I can't imagine a better OP for this excellent show.
3. Star Driver OP (Aqua Timez, "GRAVITY Ø"). Image and music combine to accelerate us into the show.
4. Dance in the Vampire Bund OP (Nakano Aiko, "Friends"). It's not the music, or the images, but the way they work together. The visual/aural rhythms are amazing, as they are in the anime itself.
5. Sore demo Machi ga Mawatteiru ED (Maids [Yazawa Rieka, Omigawa Chiaki, Yuuki Aoi, Shiraishi Ryouko], "Maids Sanjou!") -- Hilarious animation and a good comic song sung with energy, accuracy, and just the right amount of irony.
Those are my five favorites, but there are more good anime themes (links to online videos):
- Ichiban Ushiro no Dai Maou OP (Sphere, "Real Love, Real Life")
- Ore no Imouto Konna ni Kawaii Wake ga Nai OP (ClariS, "Irony")
- Tatami Galaxy OP (Asian Kung-fu Generation, "Stray Puppy And The Beat Of Rain)
- Shinrei Tantei Yakumo OP (Jangled Cat [Ono Daisuke], "Key")
- Otome Youkai Zakuro OP (Sphere, "Moon Signal" -- link to Sphere PV)).
- Giant Killing OP (The Cherry Cokes, "My Story")
- Kuragehime OP (Chatmonchy, "Koko Dake no Hanashi")
- Star Driver ED (9nine, "Cross Over")
- Shiki ED2 (Buck-tick, "Gekka Reijin").
- K-On 2 ED2 (Houkago Teatime, "No Thank You")
- Tatami Galaxy ED (Junji Ishiwatari and Yoshinori Sunahara + Etsuko Yakushimaru, "Kamisama no Yu Tori")
- Shinrei Tantei Yakumo ED (Komine Risa, "Missing You")
- Yosuga no Sora ED (Momoiro Clover, "Pinky Jones")
- Fortune Arterial ED (Veil, "I Miss You")
- Occult Academy ED (Takagaki Ayahi, "Kimi ga Iru Bashou" -- link to Takagaki Ayahi PV).