"You can't easily auto-tween a 3D rotation of a 2D character, for example."
Actually, you can. See the previous HN discussion of "Framefree", which decomposes an image into separately moving layers and uses a full mesh morph layer by layer to interpolate between frames. Some ultra-slow motion for sports is done that way.
Improving older anime, drawn at low-res and 5 FPS, has real potential. Especially if you can get better source material than old VHS tapes.