Landslides are one type of serious geological hazard which cause immense losses of local life and property. Landslide susceptibility prediction (LSP) can be used to determine the spatial probability of landslide occurrence in a certain area. It is important to implement LSP for landslide hazard prevention and reduction. This study developed a particle-swarm-optimized multilayer perceptron (PSO-MLP) model for LSP implementation to overcome the drawbacks of the conventional gradient descent algorithm and to determine the optimal structural parameters of MLP. Shicheng County in Jiangxi Province of China was used as the study area. In total, 369 landslides, randomly selected non-landslides, and 14 landslide-related predisposing factors were used to train and test the present PSO-MLP model and three other comparative models (an MLP-only model with the gradient descent algorithm, a back-propagation neural network (BPNN), and an information value (IV) model). The results showed that the PSO-MLP model had the most accurate prediction performance (area under the receiver operating characteristic curve (AUC) of 0.822 and frequency ratio (FR) accuracy of 0.856) compared with the MLP-only (0.791 and 0.829), BPNN (0.800 and 0.840), and IV (0.788 and 0.824) models. It can be concluded that the proposed PSO-MLP model addresses the drawbacks of the MLP-only model well and performs better than conventional artificial neural networks (ANNs) and statistical models. The spatial probability distribution law of landslide occurrence in Shicheng County was well revealed by the landslide susceptibility map produced using the PSO-MLP model. Furthermore, the present PSO-MLP model may have higher prediction and classification performances in some other fields compared with conventional ANNs and statistical models.