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<strong class="journal-contentHeaderColor">Abstract.</strong> Year-round continuous measurements of near-surface carbon dioxide (CO<sub>2</sub>) concentrations using in-situ trace gas analyzers were conducted simultaneously with nitrogen dioxide (NO<sub>2</sub>) measurements by International Air Quality and SKY Research Remote Sensing Network (A-SKY) Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) at Chiba (35.625° N, 140.104° E, 60 m above sea level), located within the Tokyo megacity, Japan, during 2024. These simultaneous measurements revealed that CO<sub>2</sub> concentrations were low on days when near-surface NO<sub>2</sub> concentrations were markedly reduced. Furthermore, the CO<sub>2</sub> enhancement relative to the baseline concentration determined based on such low-NO<sub>2</sub>-concentration days ([ΔCO<sub>2</sub>]<sub>N</sub>) was positively correlated with NO<sub>2</sub> and black carbon concentrations. This finding indicates that [ΔCO<sub>2</sub>]<sub>N</sub> is useful in observing the increase in fossil-fuel combustion-derived CO<sub>2</sub> within the Tokyo megacity. By employing this relatively simple method, CO<sub>2</sub> concentrations in megacities can be monitored with high accuracy and precision, contributing to more effective emission mitigation strategies.