Accurate phase constitution prediction is crucial for guiding the new steel design with desirable properties. This article uses three machine learning (ML) algorithms, backpropagation neural network (BPNN), radial basis function neural network (RBFNN), and fuzzy neural network (FNN), to compare the accuracy of predictive model. Toward the collected data, statistical measure of correlation is taken in the present work by determining Pearson correlation coefficient (PCC). The results show that the testing accuracy using BPNN is higher than the corresponding testing accuracy using RBFNN and FNN. With these understandings, the well‐known optimization algorithms, namely, mind evolutionary algorithm (MEA), are implemented to find optimal hyperparameters set that is able to induce a higher predictive capability. The resulting MEA‐BPNN further enhances the prediction results in the present dataset and efficiently explores the relationship between alloying elements and phase constitution. Finally, the reliability and practicability of the model are verified by experimental measurement on the ferrite content for prepared steels, and their mechanical properties are tested for engineering applications. As such, the work proposes a useful MEA‐BPNN model for predicting the phases of high carbon pearlite steel and provides an alternative route of designing new steels in a given system.