The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions.Because of the complex distribution of iron location on the support,the selectivity is always low.Here,we report a general strategy to selectively deposit highly-dispersed FeOx into the micropore of ZSM-5 by atomic layer deposition(ALD).The framework of ZSM-5 and the Br?nsted acid sites are intact during ALD,and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5.Besides,more Fe-O-Si bonds are formed over FeOx/ZSM-5 with a low loading of Fe,while FeOx nanoparticles are generated at high Fe loading.They cannot be realized by the traditional solution method.The obtained FeOx/ZSM-5 catalysts perform high selectivity of cyclohexanone(92%-97%),and ALD cycle numbers of FeOx control the activity.Compared with the Fe nanoparticles,the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.