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Optoelectrical Engineering In article number 2305512, Jinhyoung Lee, Taesung Kim, and co‐workers successfully present the tip‐induced optoelectrical engineering at molecular junction, which has not been previously achieved due to the critical limitations of existing spectroscopy methods. The heterogeneous interfacial charge transfer dynamics are completely revealed via synergistic correlation of photo‐induced force microscopy and Kelvin probe forcemicroscopy. It provides the interfacial tunneling control platform that enables the non‐destructive real‐time and ‐space investigation of ultra‐thin hybrid molecular junction systems.