The intrinsic structural asymmetry of Janus MoSSe offers a promising platform for stabilizing magnetic skyrmions; however, its relatively weak Dzyaloshinskii-Moriya interaction (DMI) hinders practical applications. Here, we reveal that ${\mathrm{Mn}}_m{\mathrm{Rh}}_n$ ($m+n=3$) cluster modification and strain engineering can effectively enhance both the DMI and exchange interactions by first-principles calculations. Specifically, at 4% and 6% strain, the DMI and exchange parameter ($J$) for $\mathrm{R}{\mathrm{h}}_3@\mathrm{MoSSe}$ rise significantly, reaching peak values of 4.123 meV and 18.268 meV, respectively. This enhancement stems from strain-induced modifications in the $d$-orbital distribution of Rh atoms near the Fermi level, which optimize both spin-orbit coupling and exchange interactions. Under 2% tensile strain, skyrmions with a diameter of 22 nm are stabilized in $\mathrm{R}{\mathrm{h}}_3@\mathrm{MoSSe}$. A moderate external field of 1 T reduces their size slightly to 20 nm, while a 5 T field induces the formation of 14 nm ferromagnetic skyrmions in the same system. Our findings highlight the critical role of cluster adsorption and strain engineering in modulating DMI and advancing the study of FM skyrmions in two-dimensional Janus materials.

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• Dzyaloshinskii-Moriya interaction
• Magnetism
• Janus materials
• Density functional calculations
• Skyrmions