Water-lubricated seal interfaces are particularly vulnerable to fluid-film instability, which accelerates interfacial friction and wear and compromises the reliability and service life of underwater equipment. Here, a novel graphite-microcrystalline diamond (Graphite-MCD) soft–hard seal-face tribopair was proposed and systematically benchmarked against SiC-SiC and Graphite-SiC tribopairs under high-pressure water lubrication. Their sealing capacity, friction and wear behavior, and interfacial evolution were evaluated. The polished Graphite-MCD pair achieved the highest limiting PcV (90.73 MPa·m·s⁻¹) and the lowest wear rate, markedly outperforming the SiC-SiC and Graphite-SiC pairs. Multiscale interfacial characterization showed that the SiC-SiC pair failed primarily through adhesive instability after breakdown of the water film. Although the Graphite-SiC pair reduced interfacial shear resistance, sliding generated a continuous triboreaction layer accompanied by third-body wear. In contrast, the Graphite-MCD pair preserved interfacial structural integrity and suppressed the formation of an unstable continuous reaction layer and abundant abrasive debris. This behavior enabled a synergistic combination of a low-shear lubricating interface and a stiff load-bearing counterface. These results demonstrate that improving the limiting PcV of mechanical seals cannot be achieved by reducing the friction coefficient alone; rather, it requires simultaneous control of lubricity and interfacial stability. The findings provide a mechanistic basis for designing soft–hard tribopairs for high-pressure, water-lubricated mechanical seals.