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One of the primary hurdles in microdevice fabrication lies in ascertaining the most impactful tactics for adapting metal surfaces. Through a one-pot tackle and distinct mechanochemical reactions evoked by 15 min aqueous wet sand-milling (SM-15), we successfully grafted Mo-based metal–organic frameworks (Mo-MOFs) onto graphene oxides (GOs). Following this, a convenient and readily scalable methodology of electrophoretic deposition was implemented to create controllable thickness of SM-15 GOs@Mo-MOFs lubricating films, achieving considerable enhancements of 143% and 91% in hardness and Young's modulus, respectively, when compared to those of SM-15 Mo-MOFs. The successful synthesis of SM-15 GOs@Mo-MOFs was corroborated using strategies such as x-ray diffraction, Fourier transform infrared spectroscopy, and field emission scanning electron microscopy. Analyses using the micro-tribotester indicated that the new film exhibited a lowest friction coefficient of roughly 0.5 when imposed with a load of 5 N and sliding speed of 8 mm/s. In addition, the optical profiler nano-indentation in situ scanning probe microscope revealed that SM-15 GOs@Mo-MOFs films had smaller and shallower scratches and grooves compared to SM-15 Mo-MOFs ones. The calculated results of key descriptors (EHOMO, ELUMO, ΔE, etc.) in density functional theory quantitatively disclosed the interaction mechanisms between GOs@Mo-MOFs molecules and microdevices. We first scrutinized the innate properties of molecule adsorption energy and frictional mechanical behaviors using synergetic cross-scale simulations, such as Monte Carlo and finite element methods. The expectation was that this process would motivate a valuable technique for shielding in the thriving micromanufacturing. [ABSTRACT FROM AUTHOR]