3DS has more exclusives that are good than the Vita, although Vita has a lot of games that are altogether better than what the 3DS offers.
The Vita is the better system when comparing games regardless what system said game is on. Handheld usually have a library completely filled with exclusives. Even the same games released on the handheld a lot of times was an exclusive on Nintendo consoles because it played completely different than the console and PSP version.
That's the problem with Vita being so close in power to a console is instead of getting its own games, it's getting games that the consoles are getting. Hopefully with the PS Vita TV and the the PS4 and Xbox One coming out, the Vita will get its own games rather than share games with its bigger and better PS3 brethren.
So based on all games the Vita is better, based on exclusives only, the 3DS is way better.