with regular morphology was prepared through an innovative tandem synthesis strategy for the first time, which combined the insertion of almost all aluminum sites by organotemplate-free synthesis and the sequential crystallization of residual silica sites by organotemplate-oriented synthesis. Samples with different Si and Al distributions could be synthesized by adjusting the tandem synthesis process, including temperature, time, Na 2 O/SiO 2 , etc. The obtained Si-rich-ZSM-5 and conventional C-ZSM-5 with a similar Si/Al ratio but different Al distributions, which were demonstrated by X-ray fluorescence (XRF), X-ray photoelectron spectroscopy (XPS), Transmission electron microscopy (TEM), and 1,3,5triisopropylbenzene catalytic cracking analysis, were employed in n-hexane catalytic cracking reaction. Si-rich-ZSM-5 showed a higher stability with a n-hexane conversion of 57.7% at 100 h compared with that of C-ZSM-5 (24.6%), which was attributed to its inactive outer shell. Besides, a high para-xylene selectivity in xylene for the Si-rich-ZSM-5 catalyst was obtained. Hence, this study provides a simple and cost-effective strategy to fabricate highly stable catalysts for cracking reactions.