There are many good movies and many of them listed here. I would have to second Hithcock movies. Also, as LPM mentioned Jean-Pierre Jeunet. Although I would use City of Lost Children or Delicatessen (if you can find it). The use of colors is amazing.
Also a good movie that is visually appealing is Akira Kurosawa's Dreams, but I always crash during it. It's very relaxing.
There are many more, but those are the movies I find visually nice.
Almodovar is also an excellent director if you haven't checked out any of his movies. And of course for analyzing plot, Pi or Requiem for a Dream would be interesting.
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