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The first thing that comes to mind is Little Big Planet 2. Not so you can stir up a new fanbase, but because you can find new content to suggest to the customers who buy the game.
Otherwise, I'd suggest you pick whatever games interest you. There's no point picking up, say, Crysis 2 if you're not a fan of FPS games, or Resident Evil 5 if you're not into survival horror.
What I WILL suggest is to pick some of the more obscure titles for the system that people may not immediately think of; Eternal Sonata, Marvel Superhero Squad, etc.
As for the DS, the same principles apply. Personally, I'd pick: Legendary Starfy, Final Fantasy 4, Rune Factory 3, Shin Megami Tensei Devil Survivor and, obviously, Pokemon.