I have always enjoyed Wes Anderson's soundtracks. Fantastic Mr. Fox had a great one, and Seu Jorge's Bowie covers in Life Aquatic were very excellent. Saw Moonrise Kingdom recently and it also had a good one. The part when Luke Wilson attempts suicide in Royal Tenenbaums and it is playing "Needle in the Hay" by Elliot Smith was one of the best orchestrated scenes to go along with visual / audio. Anyway, I think Life Aquatic is my favorite off the top of my head. Anderson has very good taste in my opinion.
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