Easy to get off track with opinions about the value of a set-tru chuck so before doing that I wanted to respond to the original question. No, making the register and bolt holes bigger won't turn it into a set-tru. You need 3 or 4 bolts to adjust the chuck on the backplate before locking it down to turn it into a real set-tru. On the other hand, you can do what you're thinking and possibly improve the accuracy of the chuck overall.
@darkzero does this and it seems to work for him. I do this, too, when I mount a new chuck to a backplate so I say go for it.