There are many applications with the two-phase flow of gas (hydrocarbon, non-hydrocarbon, and their mixture) and water in different courses of gas recovery from natural gas resources and gas storage/sequestration programs. As the interface of gas-water is crucial in such systems, precise prediction of gas-water interfacial tension (IFT) can aid in the simulation and development of such processes. Artificial intelligence techniques (AIT) are being used to estimate IFT. In this paper, the IFT of the gas and water system was estimated based on models built using a comprehensive data set comprised of 2658 experimental data points. These cover a wide range of input parameters, i.e., specific gravity (0.5539–1.5225), temperature (278.1–477.5944 K), pressure (0.01–280 MPa), and water salinity (0–200,000 ppm). The intelligent models include Least-Squares Boosting (LS-Boost), Multilayer perceptron (MLP), Least Square Support Vector Machine (LSSVM), and Committee machine intelligent system (CMIS). The models reproduce the IFT data in 7.4–81.69 mN/m. The modeling approaches contain new hybrid forms in which Imperialist Competitive Algorithm (ICA), Grey Wolf Optimizer (GWO), Whale Optimization Algorithm (WOA), Levenberg-Marquardt algorithm (LM), Bayesian regularization algorithm (BR), Scaled conjugate gradient algorithm (SCG), and Coupled Simulated Annealing (CSA) were used for optimization and learning purposes. Statistical and graphical analyses were implemented to check the agreement between the prediction and evaluation data. The results show a reasonable coherence for most models, among which the CMIS approach exhibited a promising performance. CMIS was accurate even in conditions of varying specific gravity, pressure, temperature, and salinity. The findings were also compared with available models in the literature and demonstrated superior predictions of the CMIS model. Also, outlier detection by the Leverage approach demonstrates the validity of the gathered dataset and, subsequently, the CMIS model.