Thank you all for your replies. I guess the bottom line is that the surface was just not prepped properly, period. Whether it wasn't primed, or whether it was primed but all the dust was not removed, we will never know. There are sparkles, kind of like a fine glitter, on the underside of the paint chips that peel off, though. That could be a clue.
I think this remodeling job occurred in the mid-eighties so low-VOC paint isn't the problem. I was also thinking that the paint failure could be due to moisture/heat issues due to the fact that the walls/ceiling are almost entirely just the underside of the roof. The other half of the attic was finished similarly in an earlier period, though, and doesn't have similar problems. But maybe it was insulated differently, or something.
ANYWAY, I think this is a job for a skilled professional. Even without this issue, the idea of painting the high, sloping walls and peaked ceiling balanced on a tall ladder is too much to contemplate... and I have an abundance of more satisfying projects I'd rather do.... so now I have a different problem..... trying to FIND that skilled professional....
I will also get some GARDZ and try it out on a limited area. If it seems like it works, my professionals, whoever they may be, may want to try it. I've read the Zinnser product info, it's an intriguing product. Thank you, BrushJockey, for your suggestions.