Modulating the magnetic properties of two-dimensional materials is crucial for advancing spintronic applications. Here, we explore the enhancement effect of perpendicular magnetocrystalline anisotropy (PMA) in $M\mathrm{T}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$ ($M$ = Pd, Pt) van der Waals heterostructures using first-principles calculations. The PMA in $\mathrm{PdT}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$ and $\mathrm{PtT}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$ is enhanced to 3.14 and 2.63 meV, respectively, more than doubling that of monolayer $\mathrm{Cr}{\mathrm{I}}_3$. This enhancement originates from three distinct mechanisms: reduced ${\left(p_{x/y}\uparrow \right)}^1\text{−}{\left(p_{x/y}\uparrow \right)}^0$ interaction gap of I atoms, magnetic proximity effect at the interface, and Rashba effect-induced modulation. Notably, $\mathrm{PdT}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$ exhibits stronger interfacial charge transfer and Rashba splitting, leading to enhanced Dzyaloshinskii-Moriya interaction. Micromagnetic simulations reveal the formation of Néel-type skyrmions under external magnetic fields, with sizes tunable from 9 nm to complete collapse at the field of 2.5 T. For trilayers, $\mathrm{PtT}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$/$\mathrm{PtT}{\mathrm{e}}_2$ shows further strengthened PMA (5.84 meV), while $\mathrm{PdT}{\mathrm{e}}_2/\mathrm{Cr}{\mathrm{I}}_3$/$\mathrm{PdT}{\mathrm{e}}_2$ exhibits spin reorientation phenomenon. Our findings provide insights into interfacial engineering of magnetic properties and demonstrate potential applications in spintronic devices.

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• Electronic structure
• Magnetic anisotropy
• Magnetic interactions
• 2-dimensional systems
• Ferromagnets
• Density functional theory
• First-principles calculations