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In the present work, Ca-induced plasticity of AZ31 magnesium alloy was studied using electron backscattered diffraction (EBSD) measurements supported by viscoplastic self-consistent (VPSC) calculations. For this purpose, alloy samples were stretched to various strains (5%, 10%, and 15%) at room temperature and a strain rate of 10^−3 s^−1. The EBSD measurements showed a higher activity of non-basal slip system (prismatic slip) as compared to that of tension twins. The VPSC confirmed the EBSD results, where it was found that the critical resolved shear stress of the various slip systems and their corresponding activities changed during the stretching of the alloy samples.