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Cu‐CHA is the state‐of‐the‐art catalyst for the Selective Catalytic Reduction (SCR) of NOx in vehicle applications. Although extensively studied, diverse mechanistic proposals still stand in terms of the nature of active Cu‐ions and reaction pathways in SCR working conditions. Herein we address the redox mechanism underlying Low‐Temperature (LT) SCR on Cu‐CHA by an integration of chemical‐trapping techniques, transient‐response methods, operando UV/Vis‐NIR spectroscopy with modelling tools based on transient kinetic analysis and density functional theory calculations. We show that the rates of the Reduction Half‐Cycle (RHC) of LT‐SCR display a quadratic dependence on CuII, thus questioning mechanisms based on isolated CuII‐ions. We propose, instead, a CuII‐pair mediated LT‐RHC pathway, in which NO oxidative activation to mobile nitrite‐precursor intermediates accounts for CuII reduction. These results highlight the role of dinuclear Cu complexes not only in the oxidation part of LT‐SCR, but also in the RHC reaction cascade. [ABSTRACT FROM AUTHOR]