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The negative thermal expansion (NTE) materials, which can act asthermal-expansion compensators to counteract the positive thermal expansion,have great applications merit in precision engineering. However, theexploration of NTE behavior with a wide temperature range has reached its upperceiling through traditional doping strategies due to composition limitations.The unique sluggish characteristic in phase transition and extendedoptimization space in recent high entropy systems has great potential tobroaden the temperature range in electronic transitions-induced NTE materials.Mn-based anti-perovskites offer an ideal platform for the exploration of highentropy NTE material due to their abundant element selection and controllableNTE performance. In this paper, the high entropy strategy is first introducedto broaden the NTE temperature range by relaxing the abrupt phase transition inMn-based anti-perovskite nitride. We propose an empirical screening method tosynthesize the high-entropy anti-perovskite (HEAP). it is found that magneticphase separation from anti-ferromagnetic CII to paramagnetic CI surviving in anultra-wide temperature range of 5K<=T<=350K (Delta_T=345K), revealing a uniquesluggish characteristic. Consequently, a remarkable NTE behavior (up toDelta_T=235K, 5K<=T<=240K) with a coefficient of thermal expansion of-4.7x10-6/K, has been obtained in HEAP. It is worth noting that the temperaturerange is two/three times wider than that of low-entropy systems. The sluggishcharacteristic has been further experimentally proved to come from disturbedphase transition dynamics due to distortion in atomic spacing and chemicalenvironmental fluctuation observed by the spherical aberration-correctedelectron microscope. Our demonstration provides a unique paradigm forbroadening the temperature range of NTE materials induced by phase transitionthrough entropy engineering.

High-Entropy Enhanced Negative Thermal Expansion Perfomance in Antiperovkites