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Monitoring of CO2 column concentrations is valuable for atmospheric research. A mobile open-path system was developed based on tunable diode laser absorption spectroscopy (TDLAS) to measure atmospheric CO2 column concentrations. A laser beam was emitted downward from a distributed feedback diode laser at 2 μm and then reflected by the retroreflector array on the ground. We measured the CO2 column concentrations over the 20 and 110 m long vertical path. Several single-point sensors were distributed at different heights to provide comparative measurements for the open-path TDLAS system. The results showed that the minimum detection limit of system was 0.52 ppm. Some similarities were observed in trends from the open-path TDLAS system and these sensors, but the average of these sensors was more consistent with the open-path TDLAS system values than the single-point measurement. These field measurements demonstrate the feasibility of open-path TDLAS for measuring the CO2 column concentration and monitoring carbon emission over large areas.