The pyrolysis of layered double hydroxide (LDH) precursors provides an effective means for designing synergetic functionalities in Cu-Mn-Al ternary nanoparticle systems. Here, a series of CuxMn2-xAl-O catalysts with LDH as the precursor were prepared and exhibited high activity for benzene combustion along with extraordinary stability and water vapor resistance. Among the tested catalysts, the Cu0.5Mn1.5Al1-O catalyst presented the best catalytic performance with the temperature required to achieve a benzene conversion of 90% (T90UUYI) at approximately 193 degrees C, which was much lower than that of the control sample, that is, CuOx-MnOx/Al2O3 (255 degrees C). The significantly improved activity was attributed to the synergistic effect between the active phases of CuOx and MnOx The increased electron density of MnOx and the weakening of the Mn-O bond in Cu0.5Mn1.5Al1-O are possible causes of the enhanced activity compared to conventional CuOx-MnOx/Al2O3. This work shows that the pyrolysis of the Cu-Mn-Al LDH precursor is a promising method for the preparation of high-performance CuOx-MnOx-based catalysts with synergistic functionality responsible for better benzene combustion activity.