Flower‐like Mo₁₅S₁₉ nanoparticles are successfully attached on the surface of the lamellar cobalt‐based zeolite imidazole framework (ZIF‐9) according to the physical mixing process herein described. The existence of lamellar ZIF‐9 not only avoids the stacking of spherical flower‐like Mo₁₅S₁₉ nanoparticles but also enhances the adsorbability of the ZIF‐9/Mo₁₅S₁₉ system for Eosin‐Y (EY) molecules, which injects more vitality into the hydrogen production reaction. In addition, the lamellar ZIF‐9 can be freely stacked and form a regular rich wrinkle structure. Benefitting from this special structure, Mo₁₅S₁₉ nanoparticles with spherical flower‐like shape can be adsorbed more firmly between the layers of ZIF‐9. This 2D/3D interlaced structure makes the system more stable, which also can improve the adsorption capacity of EY molecules. In addition, the construction of an S‐scheme heterojunction between ZIF‐9 and Mo₁₅S₁₉ is another nonnegligible driving force for the enhanced photocatalytic performance in this system. The rational establishment of the S‐scheme heterojunction provides a more convenient transmission channel for the photogenerated charge. This work uses ZIF‐9 as the carrier of Mo₁₅S₁₉ and promotes the catalytic performance of the composite ZIF‐9/Mo₁₅S₁₉ by adjusting the evacuation of the spherical Mo₁₅S₁₉ nanoparticles and constructing a heterojunction that can promote the flow ability of charges.