In this study, a polyethyleneimine (PEI)-functionalized carbon nanotube (CNT) sensor was fabricated for carbon dioxide detection at room temperature. Uniform CNT thin films prepared using a filtration method were used as resistive networks. PEI, which contains amino groups, can effectively react with CO2 gas by forming carbamates at room temperatures. The morphology of the sensor was observed, and the properties were analyzed by scanning electron microscope (SEM), Raman spectroscopy, and fourier transform infrared (FT-IR) spectroscopy. When exposed to CO2 gas, the fabricated sensor exhibited better sensitivity than the pristine CNT sensor at room temperature. Both the repeatability and selectivity of the sensor were studied.