Interface charges at atomic layer deposited Al2O3/III-nitride interfaces were investigated for III-nitride layers of different polarity. A large positive sheet charge density is induced at the Al2O3/III-nitride interface on all the orientations of GaN and Ga-polar AlGaN, and this sheet charge can be significantly altered using post-metallization anneals. It is proposed that the charges are caused by interfacial defects that can be passivated and neutralized through a H2 based anneal. Tailoring of the interface charge density described here can be used to improve critical device characteristics such as gate leakage and electron transport, and for lateral electrostatic engineering.