Fiber-reinforced self-compacting concrete (FRSCC) is a typical construction material, and its compressive strength (CS) is a critical mechanical property that must be adequately determined. In the machine learning (ML) approach to estimating the CS of FRSCC, the current research gaps include the limitations of samples in databases, the applicability constraints of models owing to limited mixture components, and the possibility of applying recently proposed models. This study developed different ML models for predicting the CS of FRSCC to address these limitations. Artificial neural network, random forest, and categorical gradient boosting (CatBoost) models were optimized to derive the best predictive model with the aid of a 10-fold cross-validation technique. A database of 381 samples was created, representing the most significant FRSCC dataset compared with previous studies, and it was used for model development. The findings indicated that CatBoost outperformed the other two models with excellent predictive abilities (root mean square error of 2.639 MPa, mean absolute error of 1.669 MPa, and coefficient of determination of 0.986 for the test dataset). Finally, a sensitivity analysis using a partial dependence plot was conducted to obtain a thorough understanding of the effect of each input variable on the predicted CS of FRSCC. The results showed that the cement content, testing age, and superplasticizer content are the most critical factors affecting the CS.