Nintendo Land. It's both Wiimote and Gamepad compatible, and has some really unique local multiplayer games, both co-op and competitive. Even some of the single player has options to let the 2nd player help with a Wiimote, kind of like Super Mario Galaxy.
Donkey Kong is a definite for co-op play. If you liked NSMBU, you could consider getting NSLU, it's a much harder expansion, but if your brother can't handle the added difficulty, he can still participate by choosing Nabbit, who is invincible to enemies. Rayman Legends is also a good option.