Hmm this might be a bit radical but what if at level 6 nunu and willump can seperate with nunu retaining an iceball skill on e, maybe some kind of root on q, and perhaps some type of shield skill on w. Willump would retain bloodboil on w, consume on q, and maybe some type of knock and or dash on e. While they are separated they can be played like two different champions and the summoner can switch between them by pressing R. Nunu can climb back on top of willump when in range of each other and upon doing so gain access to a nuke ulti in the same vein as their current ult but improved somewhat so it's not so easily countered like the current ult. While combined the player could switch between ability sets similar to jayce or nidaly.
The separation and recombination would likely take a few seconds so as to not be so op and depending on efficacy, stats could be divided between them while separated such as willump gaining the AD while nunu gets the AP and possibly a division of other stats likely in favor of willump due to his melee range and larger size.
TBH this sounds like a great way to preserve nunu's current playstyles of jungle and support while improving his effectiveness at both. I don't think it'd be very op considering he'd have to trade a significant amount of survivability post 6 to be separated as well as not having his nuke. I think itd work best if upon death the other member would stay alive, it would effectively gimp his ability for the entirety of the death timer. In cases of item effects they would be accessable to both members but go on cooldown for both upon use on one member (you wouldnt be able to build a redemption and use it once on nunu and then again on willump for example).