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The negative thermal expansion (NTE) material is counterintuitive due to itstypical feature of volume contraction on heating, which can act as thethermal-expansion compensators to counteract the normal positive thermalexpansion. A wide temperature range of NTE behavior is desired, whereas theperformance optimization by traditional doping strategy has reached its upperlimit. In this paper, the unique sluggish characteristic in high entropymaterials is proposed to broaden the NTE temperature range by relaxing thesharp phase transition in Mn-based anti-perovskite nitride. We propose anempirical screening method to synthesis the high-entropy anti-perovskite(HEAP). A remarkable NTE behavior (up to {\Delta}T = 235 K, 5 K < T < 240 K)with the coefficient of thermal expansion (CTE) of - 4.7 ppm/K has beenobserved in typical HEAP Mn3Cu0.2Zn0.2Ga0.2Ge0.2Mn0.2N, whose workingtemperature range is far wider than that of traditional low-entropy dopingsystem. The wide temperature range of phase separation due to sluggish phasetransition is responsible for the broadened NTE behavior in HEAP. Ourdemonstration provides a unique paradigm in the broadening of the NTEtemperature range for phase transition induced NTE materials through entropyengineering.

High-Entropy Anti-Perovskites with Negative Thermal Expansion Behavior