Catalytic synthesis of 2,6-dimethylphenol from methanol and KA-oil (mixture of cyclohexanol and cyclohexanone) was achieved by using magnesium oxide-supported chromium oxide catalysts in one step. The activity of Cr/MgO catalysts depended on the concentration of chromium. At high conversion (>90%), dimethylphenol was formed in high yield (>60%) with minor amounts of methylated cyclohexanol and/or cyclohexanone, which may further be reacted to form the desired product.