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Abstract The discovery of new electroactive materials is slow due to the large combinatorial chemical space of possible experiments. Efficient exploration of redox‐active chemical space requires a machine learning assisted robotic platform with real‐time feedback. Here, we developed a closed‐loop robotic platform which is capable of synthesis and electrochemical characterisation controlled using a probabilistic algorithm. This was used to probe the redox behaviour of different polyoxometalates (POMs) precursors and explore the formation of redox‐active coordination complexes. The system can run accurate analytical electrochemical measurements whilst maintaining the performance and accuracy of both the working and reference electrodes. The platform successfully ran and analysed 336 coordination chemistry reactions by performing ca. 2500 cyclic voltammetry (CV) scans for analysis and electrode cleaning. Overall, the platform carried out over 9900 operations in 350 hours at a rate of 28 operations per hour, and we identified 24 complex solutions which showed significantly different redox activity. Experiments were performed using a universal chemical synthesis language (χDL) with variable inputs. The platform was used autonomously to investigate a range of POM precursor materials demonstrating 45 % increase in capacitance. The experiments ran for 36 hours with more than 6400 operations during which we analysed 200 POM precursor solutions.