I'm assuming that you have the Adagio Multi-currency module.
You cannot change the Account Set code assigned to a vendor (or customer) that involves a change in currency code, using the user interface. You would have to create a new vendor. If you wanted to re-use the existing vendor code then you can obtain the Toolkit for Adagio (Vendor Number Changer) to change the vendor codes assigned.
Alternatively we would be happy to offer our services to change the assigned Account Sets for you.