Underground hydrogen storage (UHS) critically relies on cushion gas to maintain pressure balance during injection and withdrawal cycles, prevent excessive water inflow, and expand storage capacity. Interfacial tension (IFT) between brine and hydrogen/cushion gas mixtures is a key factor affecting fluid dynamics in porous media. This study develops four machine learning models— Decision Trees (DT), Random Forests (RF), Support Vector Machines (SVM), and Multi-Layer Perceptrons (MLP)—to predict IFT under geo-storage conditions. These models incorporate variables such as pressure, temperature, molality, overall gas density, and gas composition to evaluate the impact of different cushion gases. A group-based data splitting method enhances the realism of our tests by preventing information leakage between training and testing datasets. Shapley Additive Explanations (SHAP) reveal that while the MLP model prioritizes gas composition, the RF model focuses more on operational parameters like pressure and temperature, showing distinct predictive dynamics. The MLP model excels, achieving coefficients of determination (R2) of 0.96, root mean square error (RMSE) of 2.10 mN/m, and average absolute relative deviation (AARD) of 3.25%. This robustness positions the MLP model as a reliable tool for predicting IFT values between brine and hydrogen/cushion gas (es) mixtures beyond the confines of the studied dataset. The findings of this study present a promising approach to optimizing hydrogen geo-storage through accurate predictions of IFTs, offering significant implications for the advancement of energy storage technologies.