Photoresponsive materials for use with a volumetric additive manufacturing system are described herein. Some embodiments of photoresponsive materials described herein include at least one constituent selected from the group consisting of (i) a thiol-containing siloxane prepolymer, (ii) a vinyl-containing siloxane prepolymer, (iii) a reinforcing filler, (iv) a photoinitiator (v) a polymerization inhibitor. Methods of using the same photoresponsive materials in additive manufacturing processes such as volumetric additive manufacturing are also described.