The solubility of caffeine in water and ethanol at 0—50 ℃ was measured using the laser method. The results were regressed with an empirical equation and simplified EOS correlation. A 2-2-1 backpropagation (BP) artificial neural network (ANN) model was selected from many other models. The prediction of interpolation and extrapolation of the data was made with trained 2-2-1 BP ANN model. The result was satisfactory.