Van der Waals (vdWs) crystals have attracted a great deal of scientific attention due to their interesting physical properties and widespread practical applications. Among all, CrSiTe3 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. In this letter, we study the magnetic properties of bulk CST single crystal upon proton irradiation with the fluence of 1×10 18 protons/cm 2 . Most significantly, we observed an enhancement (23%) in the saturation magnetization from 3.9 µB to 4.8 µB, and is accompanied by an increase in coercive field (465-542 Oe) upon proton irradiation. Temperature dependent X-band electron paramagnetic resonance measurements show no additional magnetically active defects/vacancies that are generated upon proton irradiation. The findings from X-ray photoelectron spectroscopy and Raman measurements lead us to believe that modification in the spin-lattice coupling and introduction of disorder could cause enhancement in saturation magnetization. This work demonstrates that proton irradiation is a feasible method in modifying the magnetic properties of vdWs crystals, which represents a significant step forward in designing future spintronic and magneto-electronic applications. *