Landslides pose a constant threat to the lives and property of mountain people and may also cause geomorphological destruction such as soil and water loss, vegetation destruction, and land cover change. Landslide susceptibility assessment (LSA) is a key component of landslide risk evaluation. There are many related studies, but few analyses and comparisons of models for optimization. This paper aims to introduce the Tree-structured Parzen Estimator (TPE) algorithm for hyperparameter optimization of three typical neural network models for LSA in Shuicheng County, China, as an example, and to compare the differences of predictive ability among the models in order to achieve higher application performance. First, 17 influencing factors of landslide multiple data sources were selected for spatial prediction, hybrid ensemble oversampling and undersampling techniques were used to address the imbalanced sample and small sample size problem, and the samples were randomly divided into a training set and validation set. Second, deep neural network (DNN), recurrent neural network (RNN), and convolutional neural network (CNN) models were adopted to predict the regional landslides susceptibility, and the TPE algorithm was used to optimize the hyperparameters respectively to improve the assessment capacity. Finally, to compare the differences and optimization effects of these models, several objective measures were applied for validation. The results show that the high-susceptibility regions mostly distributed in bands along fault zones, where the lithology is mostly claystone, sandstone, and basalt. The DNN, RNN, and CNN models all perform well in LSA, especially the RNN model. The TPE optimization significantly improves the accuracy of the DNN and CNN (3.92% and 1.52%, respectively), but does not improve the performance of the RNN. In summary, our proposed RNN model and TPE-optimized DNN and CNN model have robust predictive capability for landslide susceptibility in the study area and can also be applied to other areas containing similar geological conditions.