In this study, an automated high-throughput Laser-driven Micro-flyer plate Impact (LMI) experimental system was used to investigate the spall strength of pure copper with grain sizes ranging from 10⁻⁹ to 10⁻⁵ m at varying strain rates and shock pressures. The samples were copper polycrystals prepared using a sputter coating methodology, with the specimens subsequently annealed to grow grains to larger sizes. The effect of crystallographic orientation on spall in single-crystal copper was also investigated. The high-throughput methodology allows for the exploration of this large parameter space. The material fabrication and experimental procedure were also automated to accelerate the exploration process. This study provides a comprehensive experimental dataset on the spall strength of copper at extremely high strain rates and discusses the necessary methodologies to automate the exploration of the parameter space.