They Might Be Giants' album for the whole family, No!, is brilliant. My son's favorite song, "Robot Parade," intones, "In a future time, children will work together to build a giant CYBORG," while my pick is the infectious, kitschy PSA "In the Middle," which gives specific instructions on how to cross the street. It's joyously entertaining for all of us.
Ronan beautifully misinterprets another track on this album, "Where Do They Make Balloons?" He sings, "Where do they make a roux?" Yes, he saw Ratatouille this summer!
TMBG have another kids' album, Here Come the ABCs. This one is not in heavy rotation at the moment, although I still myself singing, "Go, go, go go for G" more often than I'd like.
Check out GiantKid to explore TMBG's offerings for kids.