Additive manufacturing of optical, thermal and structural components require specially designed materials and advanced manufacturing processes. Building on the state of the art of laser metal deposition, this chapter describes the special challenges involved in processing copper-phosphor-molybdenum materials for additive manufacturing. Using custom experiment designs, process parameters are developed which are combined with intelligent process control. The result is the first-ever fabrication of expansion-compliant multi-material joints between yttrium aluminum garnet lasing mediums and metal materials in a single additive process.