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As part of a novel method for evolutionary material development, particle-oriented peening is used in this work to characterize 100Cr6 (AISI 52100) microparticles that were heat-treated by means of a differential scanning calorimeter (DSC). The plastic deformation of the samples in particle-oriented peening is correlated with the microstructural properties considering different heat-treatment variations. While the heating rate was kept constant (10 K/min) for all heat treatments, different heating temperatures (500 °C, 800 °C, 1000 °C and 1100 °C) were realized, held for 20 min and then cooled down at a rate of 50 K/min. Thereby, microstructural states with different (mechanical) properties are generated. For validation, microsections of the particles were analyzed and additional universal microhardness measurements (UMH) were performed. It could be shown that the quickly assessable plastic deformation descriptor reacts sensitively to the changes in the hardness due to the heat treatment.