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The usefulness of artificial neural networks for response surface modeling in HPLC optimization is compared with (non-)linear regression methods. The number of hidden nodes is optimized by a lateral inhibition method. Overfitting is controlled by cross-validation using the leave one out method (LOOM). Data sets of linear and non-linear response surfaces (capacity factors) were taken from literature. The results show that neural networks offer promising possibilities in HPLC method development. The predictive results were better or comparable to those obtained with linear and non-linear regression models.