Natural systems have evolved to provide remarkable chemical selectivity and sophisticated hierarchical structures. We propose to synthetically mimic such impressive objects through precise control over form factor, composition, and function using digital light processing (DLP), a rapid, high-resolution light-based 3D printing platform. However, resins implemented in contemporary DLP are limited to only a few reactive functionalities – acrylics/epoxies - and methods to integrate multiple components into a single print. As a MRSEC seed, we aim to overcome these shortcomings by developing novel wavelength-specific photopolymer chemistry that is reactive under exposure to low energy, visible light. Material targets that will guide our research in photopolymer resin development include structural plastics (e.g., polyesters/polyolefins) and elastomers (e.g., polyurethanes/polysiloxanes), which offer a diverse array of applications, such as soft robotics, tissue engineering, and microelectronics. Furthermore, the fundamental scientific discoveries that will stem from this seed will inform the design and development of next generation light-based soft materials and 3D bioinspired structures.