Abstract The O2-band channel configuration of existing microwave radiometers is not optimal for surface pressure retrieval, which limits the surface pressure retrieval accuracy. In this study, we present the results of theoretically what might be the optimal microwave channels for surface pressure retrieval. An improved iterative selection method is used to select the channels that contain the highest cumulative content of surface pressure information. The selected optimal channel set comprises 16 channels, among which 10 channels are centered at the 50–60 GHz oxygen absorption band and 6 channels are centered around the 118.75 GHz oxygen absorption line. Two representative spaceborne microwave radiometers are used for comparisons, the Advanced Technology Microwave Sounder (ATMS) on board the Suomi National Polar-Orbiting Partnership (SNPP) satellite and the Microwave Humidity and Temperature Sounder (MWHTS) on board the Chinese Fengyun-3C (FY-3C) satellite. The results of information content analysis show that the optimal channel set contains more surface pressure information than that of the combination of SNPP/ATMS and FY-3C/MWHTS (SNPP/ATMS+FY-3C/MWHTS) channels. A representative dataset from the ERA5 data is input into the plane-parallel Microwave Radiative Transfer model to obtain the simulated brightness temperature observations of the selected optimal channels and the SNPP/ATMS+FY-3C/MWHTS channels. Using the simulated observations, retrieval experiments are performed. Experimental results show that retrieval accuracies of the optimal channel set are 1.09 and 1.64 hPa for clear-sky and cloudy conditions, respectively. The retrieval accuracies are 0.60 and 0.65 hPa better than that of the SNPP/ATMS+FY-3C/MWHTS channels for clear-sky and cloudy conditions, respectively.