Understanding changes in terrestrial carbon balance is important to improve our knowledge of the regional carbon cycle and climate change. However, evaluating regional changes in the terrestrial carbon balance is challenging due to the lack of surface flux measurements. This study reveals that the terrestrial carbon uptake over the Republic of Korea has been enhanced from 1999 to 2017 by analyzing long‐term atmospheric CO2 concentration measurements at the Anmyeondo Station (36.53°N, 126.32°E) located in the western coast. The influence of terrestrial carbon flux on atmospheric CO2concentrations (ΔCO2) is estimated from the difference of CO2 concentrations that were influenced by the land sector (through easterly winds) and the Yellow Sea sector (through westerly winds). We find a significant trend in ΔCO2of −4.75 ppm per decade (p  < .05) during the vegetation growing season (May through October), suggesting that the regional terrestrial carbon uptake has increased relative to the surrounding ocean areas. Combined analysis with satellite measured normalized difference vegetation index and gross primary production shows that the enhanced carbon uptake is associated with significant nationwide increases in vegetation and its production. Process‐based terrestrial model and inverse model simulations estimate that regional terrestrial carbon uptake increases by up to 18.9 and 8.0 Tg C for the study period, accounting for 13.4% and 5.7% of the average annual domestic carbon emissions, respectively. Atmospheric chemical transport model simulations indicate that the enhanced terrestrial carbon sink is the primary reason for the observed ΔCO2 trend rather than anthropogenic emissions and atmospheric circulation changes. Our results highlight the fact that atmospheric CO2measurements could open up the possibility of detecting regional changes in the terrestrial carbon cycle even where anthropogenic emissions are not negligible.