I am practically in the same boat as you, auralgami. I have a bunch of 3* champs, I just champed my first 4* – IMHB (followed by X-23) – and now I’m faced with questions about what to do with upcoming ISO.
In my case, I have a fully-covered XF Wolverine at 165 and a Nick Fury with 11 covers, but I’m not planning to put ISO into either, because my Iceman and Rulk have 10 covers each, and they’re absolutely higher priority than those first two.
So my plan is:
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continue to champ an occasional 3* as they come up as rewards in PVE. I’ll be swimming in Colossus covers next week, so I might champ him. With 22 3* champs, so that’s going to happen less frequently over the next few months, so while I might champ Loki or Doom or Mystique, others like Ragnarok / Sentry / Spidey will go straight to the ISO stockpile.
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Otherwise, I’ll be diverting ISO towards Iceman and Rulk in small bits as ISO allows, so when I get my 13th cover, I won’t have to break the bank to champ them. Ideally, I’d like to take them from 133 to 200 in the next month, and hope I stumble into a few covers.
In your case, I wouldn’t champ Fury at all (or Ant-Man, IMO). I’d sit on the ISO, hope for some Rulk and Jean covers, and see what happens. Maybe you run into a streak of Th4r covers and that becomes an option. Of your remaining 3*s, the only one that jumps out at me is Torch (who I love playing boosted with IM40), but I think stockpiling ISO for the time being is the way to go.