The optimisations including and ignoring the photosensitiser TOFCO both reached maxima with the same conditions in iteration 8/10, and displayed improvement in all figures of merit included in the objective function. Compared to the intuitively selected and literature supported starting conditions that appeared high performing based on initial tests and heuristic optimisation (Table ), the holistically optimised conditions displayed 4.2-fold higher YieldCO (5.72±0.12 vs 1.48±0.24 µmol h -1 ), 57% higher TONCO (368±8 vs 249±38), 47% higher TOFCO (25±1 vs 17±2 min -1 ) and 3.8-fold higher QYCO (0.15±0.01 vs 0.04±0.01%) while SelCO was unchanged (88 vs 87±2%). This shows that systems can be optimised for high Yield, TON, TOF and QY rather than focusing on a single metric.