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1. Gold/Silver
2. Red/Blue
3. Diamond/Pearl

Gold/Silver was just made of win all around. They were just horus upon hours of relentless enjoyment. Red/Blue because they got me into the series - They had their flaws, but they were still great. Diamond/Pearl are truly worthy successors to the Pokémon series(Which I thought Ruby/Sapphire were not), but they just didn't quite make it there, I don't think.