Dissolved oxygen (DO) is a direct indicator of water pollution and an important water quality parameter that affects aquatic life. Based on the fundamental theorem of surfaces in differential geometry, the present study proposes a new modeling approach to estimate DO concentrations with high accuracy by assessing the spatial correlation and heterogeneity of DO with respect to explanatory variables. Specifically, a regularization penalty term is integrated into the high-accuracy surface modeling (HASM) method by applying geographically weighted regression (GWR) with some covariates. A modified version of HASM, namely HASM_MOD, is illustrated through a case study of Poyang Lake, China, by comparing the results of HASM, a support vector machine (SVM), and cokriging. The results indicate that HASM_MOD yields the best performance, with a mean absolute error (MAE) that is 38%, 45%, and 42% lower than those of HASM, the SVM, and cokriging, respectively, by using the cross-validation method. The introduction of a regularization penalty term by using GWR with respect to covariates can effectively improve the quality of the DO estimates. The results also suggest that HASM_MOD is able to effectively estimate nonlinear and nonstationary time series and outperforms three other methods using cross-validation, with a root-mean-square error (RMSE) of 0.20 mg/L and R2 of 0.93 for the two study sites (Sanshan and Outlet_A stations). The proposed method, HASM_MOD, provides a new way to estimate the DO concentration with high accuracy.