We present an application of a hybrid deep learning (DL) model on prediction of surface CO in China from 2015 to 2020, which utilizes both convolutional neural networks and long short-term memory neural networks. The DL model performance is better than a Kalman filter (KF) system in the training period (2005–2018). Furthermore, the DL model demonstrates good temporal extensibility: the mean bias and correlation coefficients are 95.7 ppb and 0.93 in the test period (2019–2020) over eastern China.