I don't know if continuing to grind would have made it any better. I didn't think I was going to succeed actually. .0035" is still not great, but the chuck holds work securely now, which was my primary goal.
Some things to keep in mind though:
1: I used a budget rotary tool with stone in a very janky setup...NOT a toolpost grinder.
2: The chuck jaw ways allow the jaws to tilt away from the chuck body, which afaik, cannot be changed.
3: What Keane said. Lol
4: I haven't tried to do this with the chuck that THIS thread is about. So we still have yet to see if I can get lucky twice. HA! I'll grind the snot out of it, because I don't care about the result. In fact, I should have started with it.