Developments in fiber-reinforced polymer (FRP) composite materials have created a huge impact on civil engineering techniques. Bonding properties of FRP led to its wide usage with concrete structures for interfacial bonding. FRP materials show great promise for rehabilitation of existing infrastructure by strengthening concrete structures. Existing machine learning-based models for predicting the FRP–concrete bond strength have not attained maximum performance in evaluating the bond strength. This paper presents an ensemble machine learning approach capable of predicting the FRP–concrete interfacial bond strength. In this work, a dataset holding details of 855 single-lap shear tests on FRP–concrete interfacial bonds extracted from the literature is used to build a bond strength prediction model. Test results hold data of different material properties and geometrical parameters influencing the FRP–concrete interfacial bond. This study employs CatBoost algorithm, an improved ensemble machine learning approach used to accurately predict bond strength of FRP–concrete interface. The algorithm performance is compared with those of other ensemble methods (i.e., histogram gradient boosting algorithm, extreme gradient boosting algorithm, and random forest). The CatBoost algorithm outperforms other ensemble methods with various performance metrics (i.e., lower root mean square error (2.310), lower covariance (21.8%), lower integral absolute error (8.8%), and higher R-square (96.1%)). A comparative study is performed between the proposed model and best performing bond strength prediction models in the literature. The results show that FRP–concrete interfacial bonding can be effectively predicted using proposed ensemble method.