Absolutely. Accounts can be on as many volume sets as you like. Once the account is there, create the group, and make the group's homevs= the desired volset.

You'll save alot of headaches if you pick up the volume management UDCs from Jazz. You just set up the groups/accounts you want on various volume sets in the ACCTUVOL.PUB.SYS control file and then when you do a :newgroup it'll put it on the correct volume for you.

Note that you can "move" a group to a different volume set provided it is empty of files.