Disasters have different shapes, and one of them is sudden landslides, which can put the safety of highway users at risk and result in crucial economic damage. Along with the risk of human losses, each day a highway malfunctions causes high expenses to citizens, and repairing a failed highway is a time- and cost-consuming process. Therefore, correct highway functioning can be categorized as a high-priority reliability factor for cities. By detecting the failure factors of highway embankment slopes, monitoring them in real-time, and predicting them, managers can make preventive, preservative, and corrective operations that would lead to continuing the function of intracity and intercity highways. Expansive clay soil causes many infrastructure problems throughout the United States, and much of Mississippi’s highway embankments and fill slopes are constructed of this clay soil, also known as High-Volume Change Clay Soil (HVCCS). Landslides on highway embankments are caused by recurrent volume changes due to seasonal moisture variations (wet-dry cycles), and the moisture content of the HVCCS impacts soil shear strength in a vadose zone. Soil Matric Suction (SMS) is another indication of soil shear strength, an essential element to consider. Machine learning develops high-accuracy models for predicting the SMS. The current work aims to develop hybrid intelligent models for predicting the SMS of HVCCS (known as Yazoo clay) based on field instrumentation data. To achieve this goal, six Highway Slopes (HWS) in Jackson Metroplex, Mississippi, were extensively instrumented to track changes over time, and the field data was analyzed and generated to be used in the proposed models. The Artificial Neural Network (ANN) with a Bayesian Regularization Backpropagation (BR-BP) training algorithm was used, and two intelligent systems, Particle Swarm Optimization (PSO) and Butterfly Optimization Algorithm (BOA) were developed to optimize the ANN-BR algorithm for predicting the HWS’ SMS by utilizing 13,690 data points for each variable. Several performance indices, such as coefficient of determination (R2), Mean Square Error (MSE), Variance Account For (VAF), and Regression Error Characteristic (REC), were also computed to analyze the models’ accuracy in prediction outcomes. Based on the analysis results, the PSO-ANN outperformed the BOA-ANN, and both had far better performance than ANN-BR. Moreover, the rainfall had the highest impact on SMS among all other variables and it should be carefully monitored for landslide prediction HWS. The proposed hybrid models can be used for SMS prediction for similar slopes.