Data-driven models are essential tools for the development of surrogate models that can be used for the design, operation, and optimization of industrial processes. One approach of developing surrogate models is through the use of input−output data obtained from a process simulator. To enhance the model robustness, proper sampling techniques are required to cover the entire domain of the process variables uniformly. In the present work, Monte Carlo with pseudo-random samples as well as Latin hypercube samples and quasi-Monte Carlo samples with Hammersley Sequence Sampling (HSS) are generated. The sampled data obtained from the process simulator are fitted to neural networks for generating a surrogate model. An illustrative case study is solved to predict the gas stabilization unit performance. From the developed surrogate models to predict process data, it can be concluded that of the different sampling methods, Latin hypercube sampling and HSS have better performance than the pseudo-random sampling method for designing the surrogate model. This argument is based on the maximum absolute value, standard deviation, and the confidence interval for the relative average error as obtained from different sampling techniques.