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Quantum interference (QI) plays an imperative role in the operation of molecular devices within the phase-coherent length, and it is vital to harness the patterns of QI, i.e., constructive and destructive interference. However, the size of the single-molecule device is too small compared to most gate electrodes. Those gates act like a backgate to affect the molecular component uniformly. Switching the patterns of QI in the same molecular skeleton remains challenging. Here, we develop the atomically precise gating strategy that manipulates the frontier orbitals of molecular components, achieving the complete switching of QI patterns between destructive to constructive QI and leading to a significant conductance modulation at room temperature. The chemical gating effect is exerted locally on the pyridine nitrogen through the selective interaction to cationic reagents, with which we can also control the switching reversibility …