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Depends what you'll be painting. For general flexibility (same as brush painting), the basics should include the primaries, black, and white, obviously, but I would also add a small range of browns (dark/burnt, terracotta, and a lighter tan). For wargame painting, and because the VMA versions are so nice, a range of metallics wouldn't go amiss, either.
Beyond that, I would first focus on important faction colors, if you have any. When branching out within color families, bear in mind that it's more important to get bright, highly saturated versions of colors if you want to get the most mileage from mixing - you can darken colors relatively easily, but making them brighter without turning them pastel with white? Good luck...
To round out the purchase, I'd pick up as many of the common secondary/tertiary colors as you can afford, focusing on what you expect to use most frequently. I paint a lot of green, for example, so it was well worth having a range of greens, even though I could mix them from blues and yellows. Purple, however, I use rather infrequently, so I only recently picked up a single bottle, mostly to test out a new brand.
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