A new disordered atom configuration in Fe2CrGa alloy has been created by ball-milling method. This leads to a significant enhancement of the magnetic moment up to 3.2~3.9 {mu}B and an increase of Curie temperature by about 200 K, compared with the arc-melt samples. Combination of first-principles calculations and experimental results reveals that Fe2CrGa alloy should crystallize in Hg2CuTi based structure with different atomic disorders for the samples prepared by different methods. It is addressed that magnetic interactions play a crucial role for the system to adopt such an atomic configuration which disobeys the empirical rule.
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