Efficient capture of radioiodine is essential for the protection of the ecological environment and the sustainable development of nuclear energy generation. Metal-organic frameworks (MOFs) and their derivatives provide alternative potential for overcoming the limitations of traditional iodine adsorbents. Herein this work, imidazole (Im) is dispersed into a robust mesoporous zirconium MOF PCN-222 by the heat deposition method, forming a high-uniformity composite Im@PCN-222. The large pore size and marked chemical resistance skeleton of PCN-222 allow the incorporation of Im to reach 43 wt % while surviving the chemical corrosion of activated Im. The nearly saturated loading of Im significantly benefits the sorption capability toward iodine and gives rise to an exceptional adsorption capacity of 10.04 g g-1 and excellent recyclability. This value is higher than that of most of the MOFs and their derivatives. Further, Im was also successfully deposited onto the PCN-222 functionalized porous Al2O3 ceramic filtration membrane, which endowed the hybrid membrane with efficient iodine sorption and separation properties. This work highlights a new strategy for the fabrication of the MOF-based radioiodine adsorption composite as well as MOF composite-based filters.