AbstractUnderstanding the processes, phenomena, and mechanisms occurring at the electrode/electrolyte interface is a prerequisite and significant for optimizing electrochemical systems. To this end, the advent of sub‐microsecond laser pulses has paved the way and eased the investigations of the electrochemical interface (e. g., electric double layer), which hitherto is difficult. The laser‐induced current transient (LICT) and laser‐induced potential transient (LIPT) techniques have proven to be valuable and unique tools for measuring key parameters of the electrified interface, such as the potential of maximum entropy (PME) and the potential of zero charge (PZC). Herein, we present a summary of studies performed in recent years using laser‐induced temperature jump techniques. The relation between the PME/PZC and the electrocatalytic properties of various electrochemical interfaces are particularly highlighted. Special attention is given to its applications in investigating different systems and analyzing the influence of the electrolyte components, electrode composition and structure on the PME/PZC and various electrochemical processes. Moreover, possible applications of the LICT/LIPT techniques to investigate the interfacial properties of a myriad of materials, including surface‐mounted metal‐organic frameworks and metal oxides, are elaborated.