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Team Galactic- Pokemon Diamond/Pearl
None of the villains in the Pokemon series- except for maybe Team Plasma in Black/White- have been exceptionally good. And while Team Rocket and Team Magma/Aqua were dumb in their own rights, Team Galactic from Diamond/Pearl/Platinum surpassed even them. You know what their motivation to do everything they did was? They wanted to create a new universe. That's right. With the help of the legendary duo of the Sinnoh region, Team Galactic wanted to create a new universe. They leader, Cyrus was perhaps a bit of a saving grace, but on the whole, Team Galactic has to be the worst group of villains in the Pokemon series.
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