A novel solid acid-base catalyst with aluminum and nitrogen was prepared from aluminum and amine by using triblock copolymer Pluronic F127 as a template and resol as a framework via evaporation-induced organic-organic assembly method. The catalyst was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectra. The acid-base properties of the catalyst were determined by temperature-programmed desorption using CO2 and NH3 as probe molecules, and the side chain alkylation of toluene with methanol over the catalyst has been investigated. The results show that the catalyst demonstrates the higher activity and selectivity.