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In this study, hierarchically complex hollow cage-like superstructures assembled by ZnO nanorods have been successfully constructed with water-soluble biopolymer sodium carboxymethyl cellulose as crystal growth modifiers. The number of the hollow cage could be adjusted from single-cage, double-cage, multi-cage to connected-cage. A possible formation mechanism of the hollow superstructures has also been proposed. The catalytic study shows that these ZnO superstructures have good abilities to enhance propellant combustion of ammonium perchlorate (an important oxidizer used in solid rocket propellants), by decreasing its decomposition temperature to as low as 285 °C. Photoluminescence studies reveal that the increase in the cage number leads to an increase in the relative photoluminescence intensity around 500 to 700 nm, which might be attributed to the increase in radiative defects at the interface of the components of the ZnO hollow structure with the growth in cage number.