Phase diagram and magnetic properties of Co
2 (Cr
1–xMn
x) Ga Heusler alloys were experimentally established. Single phase was obtainable in the entire composition range, 0 ≤
x ≤ 1.0. Order–disorder phase transition temperature from
L2
1 to
B2 phase (
TtL21/B2) and the Curie temperature (
TC) increased with increase of Mn composition, in other words, with increase of number of valence electrons (
Zt). The behavior of
TC is general trend in the Co-based Heuselr alloys that were systematically investigated previously, whereas the concentration dependence of
TtL21/B2 doesn't follow the Bragg–Williams–Gorsky approximation in Co
2 (Cr
1–xMn
x) Ga alloys. Spontaneous magnetization also increases with increase of
Zt with following the generalized Slater–Pauling rule, suggesting that the half-metal-type electronic structure is comparatively kept in the system.
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