A set of Mg-Cu-Al hydrotalcite-like materials with different Mg/Cu/Al ratios were synthesized by the co-precipitation technique. The prepared samples were characterized by physical techniques of XRD, FT-IR, Raman, N-2 physisorption, SEM, TEM, XPS, and UV prior to use as catalysts for the liquid oxidation of styrene. All synthesized samples possess a well crystallized hydrotalcite structure, medium surface, and uniform particles. Cu2+ ions at octahedral sites stably in the brucite-like sheets catalyze the epoxidation of styrene with tert-butyl hydrogen peroxide oxidant. The catalytic activity is related to the amount of copper content and oxidant behavior. The Cu-doped hydrotalcite catalysts show a rather good activity and high selectivity to styrene oxide (80-90%) at a high styrene conversion level. (C) 2015 Elsevier B.V. All rights reserved.