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Wario Land 3 for the US, definitely. I'd also like to see Mario Tennis, LoZ Oracle games (I wanna play them, since I never have before), and the DKC games, since I didn't get to download them before Nintendo pulled them off the Wii VC.
Also, not sure if Super Mario Bros: The Lost Level for the NES was and exception to bringing over games originally not brought over to the US (Not counting remakes of TLL), but if they were willing to bring over another game originally exclusive to Japan, I'd go with Mario Picross 2.