Polysiloxane scintillators (PSS) are of great interest due to their neutron and gamma-ray (n/γ) discrimination capability and excellent radiation hardness. However, one major drawback is their low mechanical hardness. To address this issue, we present a cross-linking agent, 1,3-diethenyl-1,3-dimethyl-1,3-diphenyldisiloxane (DS), incorporated into PSS to study its effects on various physical properties. It was found that the enhanced inter-chain entanglement of covalently bonded polymer chains by the DS cross-linker significantly improved the mechanical hardness and optical properties. Gravimetric analysis (TGA) indicated a slightl improvement in stability during thermal degradation. This cross-linker at 0-17 wt% concentrations has also slightly positive impact on the PSD performance as demonstrated by measurements of pulse shape discrimination (PSD) using a 238Pu-Be neutron source. The improved cross-linking density helped prevent both the generation of free molecule radicals and diffusion of fluorophore dyes. Consequently, the cross-linked samples remained transparent with no dye precipitation, even after 12 months of storage.