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Generation 1 obviously introduced and did the most for the series; voting for any other option would be silly.

That being said, I feel like Gold/Silver really took the Pokemon game and improved upon it in every way. World layout, gameplay, pokemon types and where they're found throughout the game, story, music, etc. It's one of the most beautiful games ever made and still my favorite pokemon experience to this day. I've slowly lost interest in pokemon every generation since then. =/

But I still play Red and Silver every so often.