Materials and manufacturing are the critical enabler of our technological world. With new materials and advanced manufacturing, new opportunities for advanced application become possible. Additive manufacturing (AM), or three-dimensional (3D) printing, is a relatively new manufacturing process, which relies on building up of parts from raw material. It reduces manufacturing waste, is flexible in part output, and opens new final part form-factors/architectures to be accessible for advanced applications. Light-based AM is well established in its ability to fabricate complex 3D structures whose unique properties exceed or are unfound in natural materials, called metamaterials. These unique 3D structures and other benefits of light-based AM make it of increasing interest for fabrication of functional devices, energy storage, sensors, and actuators among others. However, the available materials compatible with light-based AM, and AM in general, is limited. Specific material and processing limitations, viscosity, light absorption, and their underlying chemistry exclude the vast majority of materials from use in light-based AM. The majority of usable materials are on acrylic, vinyl, and thiol-based organic polymers whereas most functional materials are inorganic and not directly compatible.This dissertation focuses on the development of new materials and processes to allow the light-based AM fabrication of functional materials. This includes graphene energy storage devices, patterned 3D deposition for freeform electronics of multiple materials (conductors, dielectric, magnetic), and high-temperature ceramics for lightweight structural electronics in extreme applications. This dissertation lays the foundation for integrating light-based AM methods to electronic device applications that incorporates conducting and dielectric materials in 3D. Further development can allow advanced antenna, bioelectronics, and structural electronics.