The Disappearance of Haruhi Suzumiya
Ghost in the Shell Movies 1 & 2
The Tale of Princess Kaguya
Kara no Kyoukai
The Wings of Honneamise
End of Evangelion
I would agree if it didn't have that shit awful section filmed from a bike with wonkily added 2D.
Otherwise I'd say Hyouka and definitely DYRL; possibly Five Star Stories too.
This, although both look great, though Unicorn is let down by the CG. F91 looked pretty top tier too, especially with those Yas designs and nicely shaded mechs.
Even if the sakuga in Unicorn looks amazing, I think it looks a bit too clean and clinical. It lacks the character. The final Unicorn/NZ fight looks a bit better, but same issue.
Five Star Stories movie