A crucial factor in the efficient design of concrete sustainable buildings is the compressive strength (Cs) of eco-friendly concrete. In this work, a hybrid model of Gradient Boosting Regression Tree (GBRT) with grid search cross-validation (GridSearchCV) optimization technique was used to predict the compressive strength, which allowed us to increase the precision of the prediction models. In addition, to build the proposed models, 164 experiments on eco-friendly concrete compressive strength were gathered for previous researches. The dataset included the water/binder ratio (W/B), curing time (age), the recycled aggregate percentage from the total aggregate in the mixture (RA%), ground granulated blast-furnace slag (GGBFS) material percentage from the total binder used in the mixture (GGBFS%), and superplasticizer (kg). The root mean square error (RMSE) and coefficient of determination (R²) between the observed and forecast strengths were used to evaluate the accuracy of the predictive models. The obtained results indicated that—when compared to the default GBRT model—the GridSearchCV approach can capture more hyperparameters for the GBRT prediction model. Furthermore, the robustness and generalization of the GSC-GBRT model produced notable results, with RMSE and R² values (for the testing phase) of 2.3214 and 0.9612, respectively. The outcomes proved that the suggested GSC-GBRT model is advantageous. Additionally, the significance and contribution of the input factors that affect the compressive strength were explained using the Shapley additive explanation (SHAP) approach.