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Abstract The discovery of long-range magnetic ordering in atomically thin materials catapulted the van der Waals (vdW) family of compounds into an unprecedented popularity, leading to potentially important technological applications in magnetic storage and magneto-transport devices, as well as photoelectric sensors. With the potential for the use of vdW materials in space exploration technologies it is critical to understand how the properties of such materials are affected by ionizing proton irradiation. Owing to their robust intra-layer stability and sensitivity to external perturbations, these materials also provide excellent opportunities for studying proton irradiation as a non-destructive tool for controlling their magnetic properties. Specifically, the exfoliable Cr₂Si₂Te₆(CST) is a ferromagnetic semiconductor with the Curie temperature (T_C) of ∼32 K. Here, we have investigated the magnetic properties of CST upon proton irradiation as a function of fluence (1 × 10¹⁵, 5 × 10¹⁵, 1 × 10¹⁶, 5 × 10¹⁶, and 1 × 10¹⁸H⁺/cm⁻²) by employing variable-temperature, variable-field magnetization measurements, and detail how the magnetization, magnetic anisotropy vary as a function of proton fluence across the magnetic phase transition. While theT_Cremains constant as a function of proton fluence, we observed that the saturation magnetization and magnetic anisotropy diverge at the proton fluence of 5 × 10¹⁶H⁺/cm⁻², which is prominent in the ferromagnetic phase, in particular.This work demonstrates that proton irradiation is a feasible method for modifying the magnetic properties and local magnetic interactions of vdWs crystals, which represents a significant step forward in the design of future spintronic and magneto-electronic applications.