Two-dimensional (2D) magnetic materials provide an ideal platform for atomic-scale engineering of both structural and magnetoelectric (ME) properties. Through first-principles density functional theory calculations, we systematically investigate the magnetic and electronic properties of monolayer ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_6, {\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Se}}_6$, Janus-type ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_3{\mathrm{Se}}_3$, and ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_6-{\mathrm{MoSe}}_2$ heterostructures under vertical electric fields. Remarkably, both the Janus structure (${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_3{\mathrm{Se}}_3$) and the heterostructure $\mathrm{C}{\mathrm{r}}_2\mathrm{S}{\mathrm{i}}_2\mathrm{T}{\mathrm{e}}_6-\mathrm{MoS}{\mathrm{e}}_2$ demonstrate more than tenfold enhancement in magnetocrystalline anisotropy energy tunability compared to pristine ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_6$. This dramatic enhancement originates from symmetry-breaking effects: in pristine ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_6$ and ${\mathrm{Cr}}_2{\mathrm{Si}}_2{\mathrm{Te}}_6$ monolayers, the inherent mirror symmetry leads to cancellation of net ME responses, whereas in the engineered asymmetry in Janus and heterostructure systems, subsurface layers play a predominant role in ME effects. These fundamental insights not only advance our understanding of 2D ME phenomena but also provide a clear design strategy for developing next-generation, electric-field-tunable spintronic devices.

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• Magnetism
• Magneto-dielectric effect
• Interfaces
• Janus materials
• Density functional theory