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Honestly I'd say the Gen 5 ones are the most complementary to each other, at least design-wise. They have characteristics that create a nice dynamic but don't have such overbearing personalities that they're stuck in specific molds and they have the most varying body types/stances that really highlight their differences. It's especially noticeable if you place all (fully evolved) trios in their own groups - there's usually one that tends to stick out from the other two whereas Unova's all pop. For better or worse, they definitely work better together.
Shame about the types and gameplay.
