Anisotropic Magnetodielectric Coupling in Layered Antiferromagnetic FePS₃

We report anisotropic magnetodielectric (MD) coupling in layered van der Waals (vdW) antiferromagnetic (AFM) FePS$_3$ (N\'eel temperature $T_{\mathrm{N}}$ $\sim$ 120K) with perpendicular anisotropy. Above $T_N$, while dielectric response function along \textit{c}-axis shows frequency dependent relaxations, in-plane data is frequency independent and reveals a deviation from phonon-anharmonicity in the ordered state, thereby implying a connection to spin-phonon coupling known to be indicative of onset of magnetic ordering. At low temperature (below 40 K), atypical anomaly in the dielectric constant is corroborated with temperature dependent DC and AC susceptibility. The magnetodielectric response across this anomaly differs significantly for both, in-plane and out-of-plane cases. We have explained this in terms of preferential orientation of magnetic AFM-z alignment, implied by the in-plane structural anisotropy as confirmed by \textit{ab-initio} calculations. Controlling relative strength of magnetodielectric coupling with magnetic anisotropy opens up a strategy for tracking subtle modifications of structure, such as in-plane anisotropy, with potential application to spintronic technologies.