Accumulating electrical energy in decentralized electrical grids is a demanding task. Preliminary work exists on the charging and discharging of liquid organic hydrogen carriers (LOHCs). These carriers allow the storage of hydrogen by reversible hydrogenation of an aromatic compound. A challenge is that the chemical process has to be conducted within the power‐generating infrastructure, and therefore, continuous and fully automated implementation is mandatory. In this work, the fundamentals of controlling and automating LOHC‐based energy‐storage systems are presented. For this purpose, the identification of the controlled variable is performed before its influence on the reaction dynamics is determined. This results in a fully automated hydrogenation process, whereby the conductibility of the reaction, the performance, and the necessity of applying pressure pulsations to get a stable operation mode are shown. Derived from these results, the investigations help to establish LOHCs as feasible hydrogen carriers, which will be a decisive step to mid‐ and long‐term energy‐storage systems suitable to a modern smart‐grid infrastructure.