This study attempts to examine environmental controls of the underground CO2 concentration, taking the CO2 concentration 4 m beneath the soil as an example. An SVD-PCA-ANN (singular value decomposition-principal component analysis-artificial neural network) preview model is proposed with the data of underground CO2 concentration and 12 environmental variables (the soil and meteorological data). The R2, RMSE, and RPD values of the proposed model are, respectively, 0.8874, 0.3351, and 2.7929, performing better than the popular preview models like SAE (stacked autoencoders), SVM (support vector machine), and LSTM (long short-term memory). It is proved that the underground CO2 concentration can be approximated by a nonlinear function of the considered variables. Soil temperature, salinity, and wind speed are the leading environmental controls, which explain 32.04%, 13.68%, and 11.21% in the variability of the underground CO2 concentration, respectively. Possible mechanisms associated with the environmental controls are also preliminarily discussed.