A significant amount of NO is emitted from advanced gasoline vehicles during preheating three-way catalysts (TWCs) to operating temperature (>150°C). Pd nanoparticles (NPs) loaded on CeO2 are studied as a NO abatement material to mitigate NO emissions during the cold-start period. The air-fuel equivalence ratio is systematically switched from high to low while increasing temperature to promote NO storage below the operating temperature of TWCs and NO reduction at high temperature. Combined experimental and theoretical studies indicate that the Pd-NP–CeO2 interface modified by oxygen vacancies (VOs) plays an important role in converting NO∗ to NO2. NO2 is captured by VOs formed on the CeO2 surface, enabling the use of Pd/CeO2 as a NO storage material. Consequently, NO emission decreases by 67.6% during the cold-start period under practical conditions, which has been unattainable with conventional TWCs, thus bringing us a step closer to zero harmful emissions.