Abstract: As a mesoscale “atomic analogue”, polymer-grafted nanoparticles have the capability to self-assemble into periodic ordered superlattices, representing a novel class of condensed matter. In this study, a coarse-grained model of polymer-grafted nanoparticles coupled with Monte Carlo method is proposed to investigate the interfacial self-assembly behaviors of binary nanoparticle systems. Monte Carlo simulation results demonstrate that binary nanoparticles, through interfacial self-assembly, can form various types of superlattices such as AB, AB₂, AB₃, and A₄B₆ architectures. The type and architectures of these superlattices are effectively regulated by key parameters including interfacial interaction strength, effective radius ratio, and interparticle interaction intensity. Importantly, Monte Carlo simulation not only reproduces experimental observations of interfacial self-assembly of binary nanoparticles, but also reveal multiple previously unreported superlattice architectures.