In the low cost application of vacuum casting in rapid prototyping, a mould cavity with high modulus is necessary for producing plastics parts in small quantity. In this work, a silicone matrix was reinforced with natural fibers to improve the modulus of composites to mould and to reduce the cost of silicone materials. Sisal fiber with different compositions was reinforced with silicone in a compression moulding process. Mechanical properties were studied. An increase in tensile strength, tear strength, and better hardness was observed in sisal fiber composites . The silane-treated fiber improved the adhesion between fiber and matrix and enhanced the mechanical properties of the composites. The swelling method was adopted to determine the cross-linking density of composites through the Flory-Rehner equation. The flexibility of silicone composites decreased for higher fiber loading and there was an increase in cross-linking of the fiber network to improve modulus of the composites. A morphological study was conducted using X-ray tomography and scanning electron microscopy (SEM) to predict the defects, orientation, debonding, fractography, and interfacial adhesion of fiber/matrix composites.