Methane steam reforming is the foremost method for hydrogen production, and it has been studied through experiments and diverse computational models to enhance its energy efficiency. This study focuses on employing an artificial neural network as a model of the methane steam reforming process. The proposed data-driven model predicts the output mixture’s composition based on reactor operating conditions, such as the temperature, steam-to-methane ratio, nitrogen-to-methane ratio, methane flow, and nickel catalyst mass. The network, a feedforward type, underwent training with a comprehensive dataset augmentation strategy that augments the primary experimental dataset through interpolation and theoretical simulations of the process, ensuring a robust model training phase. Additionally, it introduces weights to evaluate the relative significance of different data categories (experimental, interpolated, and theoretical) within the dataset. The optimal artificial neural network architecture was determined by evaluating various configurations, with the aim of minimizing the mean squared error (0.00022) and maximizing the Pearson correlation coefficient (0.97) and Spearman correlation coefficient (1.00).