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(1) Background: the applications of ceramic materials in a friction pair and a moving pair are limited, just because of their poor toughness and unsatisfactory tribological characteristics. In view of this, Mo as a soft metal layer was added into a Si3N4 matrix to improve its toughness and tribological characteristics. (2) Methods: The microstructure and metal/ceramic transition layer were examined using X-ray diffraction, scanning electron microscope, electron dispersive X-ray spectroscopy, and Vickers hardness. Bending strength and fracture toughness were also measured. Tribological characteristics were obtained on the pin-on-disc wear tester. (3) Results: It can be found that the multilayer structure could improve the fracture toughness of laminated composite compared with single-phase Si3N4, but the bending strength was significantly reduced. Through microstructure observation, the transition layer of Si3N4/Mo-laminated composite was revealed as follows: Si3N4→MoSi2→Mo5Si3→Mo3Si→Mo. Moreover, the addition of the Mo interface to silicon nitride ceramic could not significantly improve the tribological properties of Si3N4 ceramic against titanium alloy in seawater, and the friction coefficients and wear rates of the sliding pairs increased with the increase in load. (4) Conclusions: The process failed to simultaneously improve the comprehensive mechanical properties and tribological performance of Si3N4 ceramic by adding Mo as the soft interfacial layer. However, the utilization of metal interfacial layers to enhance the toughness of ceramics was further recognized and has potential significance for the optimization of ceramic formulation.