Incorporating metal nanoparticles (MNPs) in metal–organic frameworks (MOFs) demonstrated great potential in the field of photo-/photothermal-catalysis. However, the oriented design and optimization of the 3D nano-architectures of MOF substrates to achieve high-efficiency light harvesting remains a challenge. Herein, guided on theoretical simulation, a facile etching strategy was employed to fabricate a 3D orderly-stacked-MOF-nanosheet-structure (CASFZU-1) with a high electric field energy-density-distribution; well-dispersed MNPs were afterwards encapsulated onto the MOF support. The unique nanosheet structure improved the light absorbance over the broadband spectrum, thereby enhancing the plasmonic photothermal effects of the MNPs@CASFZU-1 composites. Based on the plasmon-driven photothermal conversion, the MNPs@CASFZU-1 composites exhibited approximately twofold catalytic efficiency in the hydrogenation reaction and a lower temperature for the full conversion of carbon monoxide, compared to their bulk-type composites. The surface-plasmon-driven photothermal effects can be exploited in innovative MNPs@MOF platforms for various applications.