A programmable and fully automated platform is created to take over tedious manual operations in a typical catalyst development process. Synthesis and evaluation of the catalyst are coupled as an operation unit to enable continuous and unattended execution of combinatorial experiments. This platform is demonstrated in the identification of high‐performance bifunctional catalysts for water splitting from a trimetallic NiFeCo hydroxide system. The platform collects data for evaluating the performance of 66 different catalysts in oxygen evolution and hydrogen evolution reactions within a timeframe of four days. Timely feedback from the close‐coupled evaluation enables a guided focused‐area scanning of the parameter matrix, achieving both full coverage and a fine‐tuned hit with a relatively smaller number of experiments. The optimal compositions of the catalysts identified by the platform are well consistent with previous reports. Therefore, the platform is capable of generating useful data for catalyst screening, allowing a researcher to focus more on creative tasks.