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Umbrella Chronicles is more level-based, as in your character wanders down a train or through a lab and enemies jump out of the shadows at every second and you riddle them with bullets. And it has 2 player co-op.

Link's Crossbow Training is more training-based, where you stand still shoot at targets everywhere. But it does have some levels where you can walk around freely while you shoot, so that it can train newbies into mastering Metroid Prime 3 style FPS controls.

I'd go with Umbrella Chronicles. Or the Prince of Persia remake on the Wii. I think all they updated was the controls so it should be easy for him to play.