Tenet by Christopher Nolan with Remilia and Sakuya. Just to see their reactions to its take on Fate and Time (or Entropy) manipulation.
Similarly, Inception by Christopher Nolan with Doremy. Her absolutely smug look as she sees humans attempting to use the Dream-scape for their own ends will be great to watch.
Any History Documentary with Keine, for obvious reasons.
The John Wick Trilogy with Reisen and Rei'sen just so they can rate the gun-play.
The Original Alice in Wonderland with Alice Margatroid and Marisa. The former so she can think 'huh, the protagonist has the same name' and for inspiration in future Spell Cards, and the latter to tease Alice for the entire film.
This list will be updated by me editing it over time.