In no particular order:
Great Magic "Devil's Recitation" it's been said four times already
Explosion Sign "Peta Flare" (it may not be exactly pretty, but it's one attack I can't get tired of)
String Music "Storm Ensemble" (I really like this attack, it's intense but manageable, and syncs nicely with stage's theme)
Divine Virtue of Wind God (one of the best cards in all of Touhou)
Divine Light "Honour the Avoidance of Defiance" (this should have been Miko's final spell)
Resurrection Butterfly "Reflowering" (I've said it before, this card, along with the theme make up for the greatest ending in any Touhou game)