A series of HZSM-5/MCM-41 composite molecular sieves (HZM-Ns (x)) were prepared by employing nano-ZSM-5 zeolites with the SiO 2 /Al 2 O 3 ratios (x) of 50, 100 and 150 as the source. These materials were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, transmission electron microscopy, N 2 adsorptiondesorption measurement, and NH 3 temperature-programmed desorption. The catalytic cracking of endothermic hydrocarbon fuels over the HZM-Ns with ndecane as model was evaluated at atmospheric pressure and 500°C. The effect of the parent zeolite, mesopore and SiO 2 /Al 2 O 3 ratio on the structure, acidity, and catalytic performance of HZM-Ns was investigated. The HZM-Ns exhibited a skeletal matrix with nano-sized HZSM-5 particles (200-300 nm) with a controllable acidity well dispersed in and microporous-mesoporous hierarchical pores. The mesoporous structure improved the diffusion of the reactants and products in the pores, and the HZSM-5 nanoparticles uniformly dispersed in the MCM-41 matrix supplied a proper acidity, shorter channels, and a higher specific surface area for reaction. These resulted in a high catalytic activity, a high selectivity to light olefins and a long lifetime for n-decane catalytic cracking. The HZM-N (150) exhibited the excellent conversion, a high selectivity to light olefins and a long lifetime due to low diffusion resistance, high specific surface area, and appropriate acid distribution and strength, with the increasing SiO 2 / Al 2 O 3 ratio.