This study attempts to optimize the prediction accuracy of the compressive strength of high-performance concrete (HPC) by comparing data-mining methods. Modeling the dynamics of HPC, which is a highly complex composite material, is extremely challenging. Concrete compressive strength is also a highly nonlinear function of ingredients. Several studies have independently shown that concrete strength is determined not only by the water-to-cement ratio but also by additive materials. The compressive strength of HPC is a function of all concrete content, including cement, fly ash, blast-furnace slag, water, superplasticizer, age, and coarse and fine aggregate. The quantitative analyses in this study were performed by using five different data-mining methods: two machine learning models (artificial neural networks and support vector machines), one statistical model (multiple regression), and two metaclassifier models (multiple additive regression trees and bagging regression trees). The methods were developed and tested against a data set derived from 17 concrete strength test laboratories. The cross-validation of unbiased estimates of the prediction models for performance comparison purposes indicated that multiple additive regression tree (MART) was superior in prediction accuracy, training time, and aversion to overfitting. Analytical results suggested that MART-based modeling is effective for predicting the compressive strength of varying HPC age.