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Pokemon seems like the obvious answer here (though I did enjoy Pokemon Gold on the GBC and it is my 5th favorite game of all time).

I actually have much fonder memories of Kirby: Tilt 'n Tumble, strange as it may seem. I remember getting a Game Boy as a gift, and I was familiar with Kirby after playing Smash Bros. on the N64. Though gyro controls came naturally to me somehow, and it became one of my favorite handheld games that has yet to be re-released for any other platform. Sad.