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The thermal hysteresis in the cooperative spin crossover (SCO) polymer [Fe(trz)(Htrz)2]n[BF4]n (1) has been tuned by a simple ball milling grinding process. Mechanical treatment affects the size and morphology of the crystallite domains, as confirmed by multiple complementary techniques, including ESEM, DLS, and PXRD data. Upon milling, the regular cubic shape particles recrystallize with slightly different unit cell parameters and preferential orientation. This macroscopic change significantly modifies the thermally induced SCO behavio