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Composite materials that combine the unique properties of zeolitic imidazolate frameworks (ZIFs) and carbon nanotubes (CNTs) can give rise to novel applications. Here, ZIF-8/CNT composites were successfully prepared with and without the addition of an agent template. The size of the ZIF-8 crystals in the composite materials was controlled by varying the template, feeding order, and concentration of reactants. Thus, ZIF-8 crystals with a wide variety of sizes (from nano- to micrometer size, which is range that differs by a factor of 10) were obtained, depending on the conditions. This size-controllable synthesis of ZIF-8 was achieved by modifying the number of nucleation sites on the CNTs, as revealed by density functional theory (DFT) calculations. This work provides an efficient method for preparing ZIF-8/CNT composites with controllable size and can pave the way for the synthesis of other metal-organic framework (MOF)/CNT composite materials.