YES I would love card games so much. Bucky would first need to be retaught how to play cards (idk if you're canon familiar but brainwashing: it's a problem, he doesn't remember much except murder atm), but it's something he'd probably be curious enough about to poke his nose in if people around him are playing! He'd be bad at it first but maybe eventually scary good at poker due to being really hard to read when he's not emotionally invested.

I'm not sure Bucky would be a good candidate for helping encourage Captain to plug into the Matrix, just because he's such a concrete thinker he's going to have trouble conceptualizing the rules of physics as flexible in the Matrix, and therefore I don't think he'd latch onto Captain's potential usefulness very easily on his own steam. However, I would love to have him help/attempt to help train Captain in more concrete operative skills later down the line! Bucky is a not liable to be a gentle trainer, but he's good for line-facedly tolerating other people's antics and patient enough to wait for people to come around to learning.