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A framework of compositionally graded Ti-Al alloys was proposed to elucidate the Al alloying depen-dent deformation mechanism at room temperature.Slip trace analysis demonstrated low-alloyed Ti-Al model materials were plastically deformed by prismatic slip,pyramidal slip,stacking faults,and defor-mation twins.Increasing Al concentration promoted chemical ordering,thus suppressing the dislocation motion and deformation twinning.The mechanism behind such a kind of composition-mediated defor-mation physics was discussed.Our findings are expected to be applicable in the design of next-generation high-performance structural materials through the tailoring of the chemical ordering of solute atoms in substitutional solid solution.