Depends on genre, I'm really bad at choosing a favorite series.
It'd probably go something like
Series:
Evangelion (waiting for the next film to decide whether I prefer the series including The End of Evangelion or the new reboot films)
Toradora! (I know, I know)
Soul Eater/Death Note/FMA:Brotherhood (Can't choose, love all three)
Films
The Girl Who Leapt Through Time (Joint 1st)
The Disappearance of Haruhi Suzumiya (Joint 1st)
Gintama Film
Redline