The corrosion of steel reinforcement necessitates regular maintenance and repair of a variety of reinforced concrete structures. Retrofitting of beams, joints, columns, and slabs frequently involves the use of fiber-reinforced polymer (FRP) laminates. In order to develop simple prediction models for calculating the interfacial bond strength (IBS) of FRP laminates on a concrete prism containing grooves, this research evaluated the nonlinear capabilities of three ensemble methods—namely, random forest (RF) regression, extreme gradient boosting (XGBoost), and Light Gradient Boosting Machine (LIGHT GBM) models—based on machine learning (ML). In the present study, the IBS was the desired variable, while the model comprised five input parameters: elastic modulus x thickness of FRP (EfTf), width of FRP plate (bf), concrete compressive strength (fc′), width of groove (bg), and depth of groove (hg). The optimal parameters for each ensemble model were selected based on trial-and-error methods. The aforementioned models were trained on 70% of the entire dataset, while the remaining data (i.e., 30%) were used for the validation of the developed models. The evaluation was conducted on the basis of reliable accuracy indices. The minimum value of correlation of determination (R2 = 0.82) was observed for the testing data of the RF regression model. In contrast, the highest (R2 = 0.942) was obtained for LIGHT GBM for the training data. Overall, the three models showed robust performance in terms of correlation and error evaluation; however, the trend of accuracy was obtained as follows: LIGHT GBM > XGBoost > RF regression. Owing to the superior performance of LIGHT GBM, it may be considered a reliable ML prediction technique for computing the bond strength of FRP laminates and concrete prisms. The performance of the models was further supplemented by comparing the slopes of regression lines between the observed and predicted values, along with error analysis (i.e., mean absolute error (MAE), and root-mean-square error (RMSE)), predicted-to-experimental ratio, and Taylor diagrams. Moreover, the SHAPASH analysis revealed that the elastic modulus x thickness of FRP and width of FRP plate are the factors most responsible for IBS in FRP.