The objective of this paper is to create a new artificial neural network (ANN) model to predict solubility of CO2 in a new structure of task specific ionic liquids called propyl amine methyl imidazole alanine [pamim][Ala]. Equilibrium data of CO2 solubility were measured at the temperatures of 25, 40, and 60 degrees C and the pressures up to 50 bar. For the purpose of performance comparison, the two most common types of ANNs, multilayer perceptron (MLP) network and radial basis function (RBF) network were used. Water content, ionic liquid content, temperature, and pressure set as input variables to ANN, while CO2 capture rate assigned as output. Based upon optimization process, MLP neural network with 14 neurons in the hidden layer, log-sigmoid transfer function in the hidden layer and linear transfer function in the output layer, exhibited much better performance in prediction task than RBF neural network with the same neuron numbers in the hidden layer. Results obtained demonstrated that there is a very little difference between the estimated results of ANN approach and experimental data of CO2 capture rate for the training, validation, and test data sets. Furthermore, Henry's law constants were obtained by fitting the equilibrium data.