Titanium ALPOs, TAPO-5, TAPO-11, and TAPO-36, which have been synthesized hydrothermally, were found to be active in cyclohexane oxyfunctionalization, cyclohexanol and 2-hexanol oxidation, and octene-1 and cyclohexene epoxidation in the presence of dilute hydrogen peroxide. TAPO catalytic oxidation activity was shown to be associated with framework-incorporated Ti atoms and not with any hypothetical Ti species in reaction solution. This activity and H2O2 selectivity were in the order TAPO-5 > TAPO-11 > TAPO-36, with TAPO-5 being only slightly less active and selective than a titanium silicalite (TS-1) sample of similar Ti content and higher BET surface area.