For Wii originals, I'd say go for Rayman Raving Rabidds and Prince of Persia: Rival Swords.
As for Virtual Console titles, if you live in America get Super Metroid and Super Mario 64, if not, get Wonderboy in Monsterworld and Super Mario 64.
I've also heard that LYlatwars/Star Fox 64 is pretty good as well.
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