Through in silico studies, we showed the scalability of our approach in handling large batch sizes of 96 and high-dimensional reaction search spaces of 530 dimensions. We also assessed the robustness of our workflow to chemical noise and accommodated for batch constraints typical in chemical laboratories, demonstrating its suitability for real-world applications. We applied our approach experimentally through an automated 96-well HTE optimisation campaign for a nickel-catalysed Suzuki reaction, exploring a search space of 88, 000 possible reaction conditions. Our optimisation workflow identified reactions with an area percent (AP) yield of 76% and selectivity of 92% for this challenging transformation, whereas two expert-designed HTE plates failed to find successful reaction conditions. This study demonstrated advantages of our approach over traditional, purely experimentalist-driven HTE plate design, highlighting its potential to accelerate automated reaction optimisation. The 672 HTE reactions conducted in this study are made available in the Simple User-Friendly Reaction Format (SURF) with the custom code used in an open-source code repository, Minerva.