Although essentially every game on this list deserves to be run, I would like to place a sole vote on Chrono Twins.
Rockin' Kats - I agree that this game could probably be optimized much more, and that it could make for a good competition to see how much it can be improved, but I don't buy into the belief that this will never be re-run if we don't do it here. Games that have been published before have a much higher chance of being run than an obscure game with little to no resources or recognition in the TAS community. Furthermore, improvements are not something that I believe can be rushed. With the other games, we are going in blind and we have no idea how long the movies will end up being, so we have no standard to meet. With an improvement, our goal is to focus on every single flaw done by the previous author; this simply can't be done well in the given time restraints.
Crouching Tiger, Hidden Dragon - I honestly found nearly no information on this game. Although I'm sure this is a good game, we have enough alternatives for me to overlook this.
Captain Commando - The only real reason I like this idea is because the game is where the name Capcom came from (
Captain
Commando). We already have a 4-player beat-em-up on this site (
The Simpsons), and I doubt its quality can be matched in the given amount of time.
Sorceror's Maze - Looks really cool, but it's breakout clone that seems like it will take significantly longer than all of the other games. I'm sure this will become repetitive after a while for the viewer, even if I'm sure it'd be fun to TAS.
Chronos Twins - Wow, what's not to like? A DS game without touch screen input, and one with an interesting concept at that. This is similar to a multi-game run, but with a connection between the two games. It would have all the entertainment of a multi-game run, except it would have an actual connection, and it wouldn't have redundant sounds all going on at once. Best yet, when you're actually playing this game, I'm sure you have to stop and think about what's going on in each world; in TAS, this hesitation is removed, inevitably making the final product incredibly impressive. I also don't believe this game will get the same level of attention anywhere outside of this contest, due to it not being well known (This is the first time I've ever heard of it, at least). I've never tried TASing on the DS, and I'd probably be much more comfortable running a NES game (Especially considering it might lead to another verification), but this game is so interesting that I cannot in good conscious hurt its chances of being the chosen game by voting for anything else.
But hey, that's just my two cents. I'll be happy running any of these, mostly because none of them are for the Genesis (I hate Gens).