A one-step synthesis of cyclohexanone acetals from phenol/alcohol mixtures has been explored using bifunctional aluminum borates supported Pd catalysts. Three aluminum borates have been prepared via either a high temperature calcination (9Al(2)O(3)center dot 2B(2)O(3)) or a self-pressured thermal synthesis (PKU-1 and ABO-X) using various aluminum precursors and boric acid. Well dispersed Pd nanoparticles loaded on these materials show excellent phenol hydrogenation activity in both water and ethanol. The reactivity follows the trend of Pd/ABO-X > Pd/9Al(2)O(3)center dot 2B(2)O(3) > Pd/PKU-1, which is similar to the sequence of BO4/BO3 ratio presented in the aluminoborates as shown by NMR spectra. When ethanol is used as a solvent, 13.5 % yield of cyclohexanone diethyl acetal has been obtained under the conditions investigated on Pd/ABO-X, which is attributed to its high activity in both hydrogenation and acetalization for the one-step synthesis of cyclohexanone acetals.