Sounds like The Museum Company to me.

Oop! was over where the Verizon store is now (if that's still there, I haven't been to the mall in years) and they were more of an eclectic americana folk art / global village coffeehouse aesthetic than educational toys and the like. Lots of tchotchkes, gag gifts, ironic magnets, one off furniture, and glass art. Frog and Toad reminds me of that store, somewhat.

Perhaps you're conflating the two or I'm just forgetting some of the other products they sold, but your description definitely reminds me of The Museum Company.

Edit: after googling I think it was The Discovery Channel Store.

I miss Oop! in either case.