In LO LOC and HI LOC, the front driveshaft should spin all the time, even with the hubs in FREE.
Yes, don't go into neutral unless the engine is off or you are in PARK.
I would start by liberally dousing the shifter box with something like Silikroil or PBBlaster, to make sure nothing is stuck in the shifter itself. You can just pour it all over it from the top through the shifter hole in the floor, and see if it frees up. Mine is easy to shift back and forth through all five positions. If the 4 LOCK light doesn't come on in HI LOC, then the LOCK lever to the NP203 is not moving far enough to engage HI LOC.
You could have a busted chain packed up in the NP203 or something drastic like that, but it may just be a balky shifter box.