[mac2612] has developed a custom retroarch-based firmware for the Leapster GS and LeapPad2. (via Bringus Studios on YouTube) We covered Linux on the Leapster before, but Retroleap seems better ...
However, you could totally get away with using other systems as well like Lakka or just plain RetroArch. If you want to get a closer look at this Raspberry Pi project in action, you can check it ...