I think that they shouldn't have the infinite since infinites suck, but it should be done in a way that doesn't take away from the CG. What I mean is that if you made it escapable, people would just use that escape everytime they got grabbed and not fear the grab.
If they made it only go for only a certain amount of grabs it would become repetitive and the same grab combo each time (although thats a viable option), so I think the best way to deal with it is to make IC's grab combo's more dynamic and act a little like the other combos done in game.
A solution I'm thinking of is to make Nana's grab auto-upthrow (ends combo but still leads to a possible follow up) so that the player relies on different Popo regrab setups to keep the combo going, each one escapable through a different method that doesn't work against the other setups.
That way an IC grab would work the same way most combo starters worked where the opponent can DI in either direction and the player has to follow based on the opponent's DI to either extend the combo or finish.
Here's how I think this could work:
Like I already said make Nana's grab auto-upthrow, thus removing one of the infinites, but making for a decent finisher (up-throw might need to be changed for that purpose, maybe just Nana's throw).
The Popo:Dthrow - Nana: Fair - Popo: Ice Block - regrab infinite could be fixed by making Nana's Fair hit at a more forward trajectory so the block can't hit them in time, turning it into a finisher (also passively buffing it as a spike since forward-down is just a bit sexier than just down)
For Popo regrab setups (I actually put a lot of thought into how this could work), a few edits would make some of them easily possible:
If Popo's grab attack was changed so that he lets go if the opponent gets hit during it (not sure if that edit is doable yet, but I think this would be sick), and Nana's jab had super-armor frames (sounds absurd, but it'd really have no other effect outside of grab setup)
that opens up the possibility for grab-attack - Nana: jab - regrab, can be spot dodged (roll is too slow) or interupted (grab or a fast jab) if they react fast enough
if they jabbed or dodged, they eat a Nana grab-upthrow if you were trying to grab
if they jabbed or grabbed and you predicted, they eat a Nana Fsmash or Dsmash
if they dodged and you predicted, you wait till the dodge ends and when they come out, you make them your B!@tch
If those edits can't be done yet, there's still other ones that could be done to make the IC's grab into something new and dynamic while still keeping the same vibe that the IC chaingrab is supposed to have.