This thesis outlines the development of new elastomeric materials and manufacturing processes for soft robotics. Specifically, this work describes the development of custom material formulations for use in additive manufacturing, additive manufacturing processing techniques for silicone elastomers, and multi-component additive manufacturing techniques. Material synthesis and processing is a gap in the field that needs more research to produce more predictable, higher quality, and more scalable soft robot technologies. This thesis includes papers that address the above topics, preceded by an introduction and literature review into additive manufacturing and materials characterization for soft robotics. The first work (Chapter 2) outlines the development of a custom elastomer designed to make biodegradable soft robots via 3D printing. The second work (Chapter 3) shows how liquid silicone thermoset polymers 3d printing can be improved by controlling reaction kinetics and rheology. The last work (Chapter 4) describes the process of using silicone 3D printing to embed multiple discrete sensing and electronic components into a functioning soft wearable device, with a focus on customizability. Each work describes a different part of how materials science plays a role in soft robotics, including the creation of elastomeric material, control of the elastomeric material, and combining the multiple materials in custom device manufacturing. For each work, a soft robot actuator or robot system is developed to emphasize the importance of material behavior and process development in improving soft robot manufacturing.