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Enhancement of the low-temperature (LT) performance of selective catalytic reduction (SCR) of NOx with NH3 has been a spotlight in environmental catalysis. Here, we use a bifunctional catalytic system mixing V–W/Ti with an oxidative component, i.e., MnOx/CeO2, to achieve both improved LT-SCR activity and N2 selectivity. An integrated approach of steady-state kinetic measurements, chemical trapping techniques, time-resolved in situ FTIR spectroscopy, and density functional theory (DFT) calculations reveals that such a synergistic enhancement is at a short distance and is significant when V–W/Ti and MnOx/CeO2 are in intimate contact. These findings further suggest a bifunctional LT-SCR pathway mediated by a short-lived, mobile nitrite-precursor intermediate, which is facilely generated on the oxidative component and then communicates with the adjacent SCR phase through reacting with the abundant NH3 adsorbates there. Assembling such a mechanism with commercial SCR catalysts, accordingly, acts as a promising way to enhance the LT-SCR performance.