Good stuff.
Some notes:
Smeesh likes Raptor Boost a LOT. The vast majority of the times where he did a cross-up aerial on your shield, he would follow it up with a raptor boost, regardless of what percentages you were at. When at low percentages, an easy way to beat this is to just drop the shield after the cross-up aerial and then CC -> grab the raptor boost. He'd also just throw the move out on a lot of random occasions; to beat that, CC is again an option, although it's risky if you have a hard time shield knees/stomps on reaction, in case he chooses to do one of those instead. Another easy way to beat raptor boost is to just wavedash backwards when you think he might do it, since the move will just miss and you can punish it however you like.
I know I've told you this a million times, but light-shielding a little more often would help. The regular shield is actually pretty solid against Smeesh since he goes for a lot of stuff that can be shield-grabbed out of it, but when your shield is too small too reliably protect you against knees and stomps, you should consider busting out the light-shield; there was at least one shield-poke knee in that set that really shouldn't have happened.
Your grabs generally didn't accomplish as much as they should have. Sometimes, this was because you'd continue going for CGs even at percentages where a charged usmash or fsmash would KO. On one occasion, you were doing a handoff to him and messed up because you were trying to not move very far forward with each successive grab. It's fine to do that if you know you can consistently do it, but I think it's generally better to just walk quite a bit forward with each Popo grab since it's much easier not to mess up that way and the damage done is still very good. Kind of a minor note, but if you've grabbed someone at a high percentage and you're waiting for Nana to get back in sync and it's not clear if she'll get there in time, do dthrow with Popo. Since the dthrow animation on Falcon is quite long, it might buy you some extra time that you wouldn't have had otherwise.
Other than that, you generally looked pretty solid. You might want to practice spacing uair -> aerial combos since you missed a few of those for no apparent reason, but I didn't see any really glaring flaws with how you approach the Falcon match-up.