While the beneficial physical properties of silicone polymers are exploited in many sustainable applications, the high energy requirement for their synthesis compromises to a degree their sustainability. We report a strategy to mitigate this issue by filling the silicone with inexpensive and renewable starch. Elastomeric materials with covalently grafted starch, utilizing anhydride-modified silicones, permits loading of up to about 75% starch while maintaining many of the properties of the silicone. Alternatively, 50 wt.% starch-filled silicone foams can be prepared simply by mixing powdered starch with a mixture of HSi-functional silicone fluids in the presence of B(C6F5)3. The physical properties of the resulting foams are determined by the quantity of SiH, which controls the final density of the foams (ranging from 0.258–0.875 g mL−1), their Young’s modulus, and their degree of elasticity; both rigid and flexible foams were prepared. Materials with a high natural and renewable material content better adhere to green chemistry principle 7, should enhance the ease of degradation at end of life, and augment the sustainability of these silicone composites.