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Haven't seen all of the movies, but from the ones I have watched I would say Rise of Darkrai, since it featured three of my favourite legendaries in Darkrai, Palkia and Dialga
I loved this one too, since Diancie was so sweet and cute! hardly see anyone mention it in their favorites ;_;
for me, probably Heroes, Lucario, and Spell of the Unown... though I am biased and liked most of them. Jirachi's was another great movie with a lovely soundtrack/story.