Apparently there's a rumor regarding Devil's Third becoming a WiiU exclusive, but I haven't checked it yet. I think it would be a good move, given how the game has an acclaimed developed behind it (Itagaki) and is the kind of game that can attract a good number of the self-proclaimed "hardcore" gamers that currently doubt the WiiU. It would complement Bayonetta nicely, with its own set of attributes to distinguish it (online multiplayer, TPS elements, a more Western flavor when it comes to aesthetics, etc). Given how, as far as we know, it's still without publisher... It's quite possible.
Another possibility is the new Darkstalkers... If the platform isn't decided yet... Seems that Ono has been struggling with its development because of being unable to fully convince Capcom of its sales potential. Getting an exclusive fighter from Capcom would be quite helpful for WiiU in this area, and I don't think it would cost a lot. Getting it as a timed one is not out of the question either.
Shenmue 3 would win the heart of thousands of gamers by itself and a lot of... Let's call it, "hardcore credit" ^_^ . Even more than Bayonetta, considering the current status of the franchise. The problem with it is that it would be a very expensive project, so it's doubtful whether is worthy or not. One thing Nintendo could do would be to arrange an exclusive, retail release of Shenmue I and II in HD (and with a Japanese VA option !), in order to measure its sales potential. Getting Yu Suzuki on board wouldn't be hard as he apparently would love to work on a 3rd game, but the question is which developer team would work with him... Perhaps the Yakuza team ? That could work...
Beyond Good and Evil 2 is another option for sure, but it has a similar problem to Shenmue 3. A very expensive project with dubious rewards. So I don't think it would be cheap to get it as a full exclusive. Maybe as a timed one... That would be feasible. That aside, I don't think that Ubisoft would accept it anyway, as they seem to be decided on a multiplatform release.
There's also Mega Man Legends 3... And that's all I have to say about that...
Then of course you can come up with a ton of classic franchises with plenty of potential that for one reason or another haven't gotten a new game for while... How about a new Chrono game ? Breath of Fire ? Mana ? Onimusha ? Maybe something a bit more niche and less costly like Bloody Roar, Bushido Blade or even Gradius (as a digital download by Treasure ?). There's clearly a lot to choose from, not to mention any new concept that wanders around...
In any case, I think the whole idea of looking into the development of exclusive games that lack financial support to be made despite being from acclaimed franchises/developers is definitely great, for both Nintendo and us, gamers. It's not the only way to gather 3rd party support, but surely the most effective. It just needs to be done carefully and not on a lot of projects, just the ones that truly justify it and/or aren't much of a gamble. You can't let 3rd party publishers get used to this kind of financial support on a regular basis because then it could make their whole support dependant on it, nor can you take big financial risks on satisfying a small set of gamers. Everything in moderation. Oh, and let's not forget that Nintendo needs to invest on its own IPs too ! (and actually localize them !)