Metal halide perovskites are a promising class of materials for next-generation photovoltaic and optoelectronic devices. The discovery and full characterization of new perovskite-derived materials are limited by the difficulty of growing high quality crystals needed for single-crystal X-ray diffraction studies. Additionally, the toxicity and chemical instability of lead containing perovskites affects their commercial viability.  As such, non-lead containing systems have been the focus on considerable interest in recent years.  We present an automated, high-throughput approach for copper halide perovskitoid single crystal discovery, based on an antisolvent vapor diffusion crystallization route.  The high-throughput experimental route, and associated results, are presented as a means to rapidly identify and optimize synthesis conditions for the formation of high-quality single crystals.  A series of new compounds were discovered, including both copper halide perovsketoids and alternative hybrid materials. Analysis of the crystallization fields for each compound enabled the elucidation of formation principles that govern their formation, including reactant concentrations and the formation of hydrogen-bonding networks.