LAUSR

A robust single‐molecule memristor is prepared by covalently integrating one phenol molecule with multiple binding sites into nanogapped graphene electrodes. Multilevel resistance switching is realized by the electric‐field‐manipulated reconfiguration of the acyl moiety on the phenol center, that is, the Fries rearrangement. In situ measurements of the reaction trajectories with an initial single substrate and an intermediate break through the limitation of macroscopic experiments, therefore unveiling both intramolecular and intermolecular mechanistic pathways (a long‐term controversy) as well as comprehensive dynamic information. Based on this advance, high‐performance single‐molecule memristors in both the solution and solid states are achieved successively, providing a new understanding of memristive systems and neural network computing.