the whole drive is great. Doing the beartooth highway is great, but if you do the more southern route Cody is a fun place to visit as well. They have a lots of great museums, including one in an LDS chapel, and rodeos every night in the summer.
Driving over the Bighorns is beautiful. Devil's tower is cool and only take a few hours. Once you get to the black hills there are lots of hikes (Sylvan Lake is easy and really pretty), Custer State Park, Wind Cave Nat'l Park, and take your kids to Reptile Gardens.