try doing what JLD suggested. i would try it on a straight, less traveled road. a helper would be handy to get out and look from the side of the road at the drive shafts. come to a stop, get out, lock the hubs, shift the truck into N, then hit the button for 4Lo. put it in drive, then sense for the thunk. then try 4Hi.
this way you can eliminate the transfer case from being 'bad'
do you exercise 4WD in the 'off season'. could just be sticky.
the servo in the transfer case might be suspect, but i think its unlikely.