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Carbon dioxide (CO₂) is one of the main greenhouse gases leading to global warming, and the ocean is the largest carbon reservoir on the earth that plays an important role in regulating CO₂ concentration on a global scale. The column-averaged dry-air mole fraction of atmospheric CO₂ (XCO₂) is a key parameter in describing ocean carbon content. In this paper, the Data Interpolation Empirical Orthogonal Function (DINEOF) and the Bayesian Maximum Entropy (BME) methods are combined to interpolate XCO₂ data of Orbiting Carbon Observatory 2 (OCO-2) and Orbiting Carbon Observatory 3 (OCO-3) from January to December 2020 occurring within the geographical range of 15–45°N and 120–150°E. At the first stage of our proposed analysis, spatiotemporal information was used by the DINEOF method to perform XCO₂ interpolation that improved data coverage; at the second stage, the DINEOF-generated interpolation results were regarded as soft data and were subsequently assimilated using the BME method to obtain improved XCO₂ interpolation values. The performance of the synthetic DINEOF–BME interpolation method was evaluated by means of a five-fold cross-validation method. The results showed that the Mean Absolute Error (MAE), the Root Mean Square Error (RMSE), and the Bias of the DINEOF-based OCO-2 and OCO-3 interpolations were 2.106 ppm, 3.046 ppm, and 1.035 ppm, respectively. On the other hand, the MAE, RMSE, and Bias of the cross-validation results obtained by the DINEOF–BME were 1.285 ppm, 2.422 ppm, and −0.085 ppm, respectively, i.e., smaller than the results obtained by DINEOF. In addition, based on the in situ measured XCO₂ data provided by the Total Carbon Column Observing Network (TCCON), the original OCO-2 and OCO-3 data were combined and compared with the interpolated products of the synthetic DINEOF–BME framework. The accuracy of the original OCO-2 and OCO-3 products is lower than the DINEOF–BME-generated XCO₂ products in terms of MAE (1.751 ppm vs. 2.616 ppm), RMSE (2.877 ppm vs. 3.566 ppm) and Bias (1.379 ppm vs 1.622 ppm), the spatiotemporal coverage of XCO₂ product also improved dramatically from 16% to 100%. Lastly, this study demonstrated the feasibility of the synthetic DINEOF–BME approach for XCO₂ interpolation purposes and the ability of the BME method to be successfully combined with other techniques.