We report experimental and theoretical studies of defects producing fixed charge within Al2O3 layers grown by atomic layer deposition (ALD) on In0.53Ga0.47As(001) substrates and the effects of hydrogen passivation of these defects. Capacitance-voltage measurements of Pt/ALD-Al2O3/n-In0.53Ga0.47As suggested the presence of positive bulk fixed charge and negative interfacial fixed charge within ALD-Al2O3. We identified oxygen and aluminum dangling bonds (DBs) as the origin of the fixed charge. First-principles calculations predicted possible passivation of both O and Al DBs, which would neutralize fixed charge, and this prediction was confirmed experimentally; postmetallization forming gas anneal removed most of the fixed charge in ALD-Al2O3.