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The influence of Cu doping on phase transition, thermal strain, and thermal expansion property of polycrystalline Ni50Mn23−xCuxGa27(x = 1, 3, 5, 6 and 7) alloys is investigated. The results show that with increasing Cu concentration, martensitic transformation gradually gets close to Curie transition. A magnetostructural transition (MST) is observed in samples with x = 6 and 7. Such MST can enhance magnitude of transformation strain. Besides, Ni50Mn23−xCuxGa27 alloys possess an isotropic, recoverable, and thermally stable thermal strain. Excitedly, Cu doping can effectively tune the phase transition, thermal strain, and thermal expansion properties of Ni50Mn23−xCuxGa27 alloys. Adjustable coefficients of thermal expansion from positive to negative are obtained by Cu‐doped Ni50Mn23−xCuxGa27 alloys. The average linear expansion coefficient (α) between −140.44 and −207.70 ppm K−1 is observed in samples with x = 6 and 7 for a narrow temperature span of 11–14 K. When the temperature span is about 72 K (x = 6) and 73 K (x = 7), which is the largest temperature span observed in Ni–Mn–Ga‐based alloys recently, the α values decrease to about −36 ppm K−1. These findings are beneficial for manipulating the thermal expansion property of Ni–Mn–Ga–Cu alloys and their multifunctional applications. [ABSTRACT FROM AUTHOR]