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The charge, spin, and composition degrees of freedom in high-entropy alloyendow it with tunable valence and spin states, infinite combinations andexcellent mechanical performance. Meanwhile, the stacking, interlayer, andangle degrees of freedom in van der Waals material bring it with exceptionalfeatures and technological applications. Integration of these two distinctmaterial categories while keeping their merits would be tempting. Based on thisheuristic thinking, we design and explore a new range of materials (i.e.,dichalcogenides, halides and phosphorus trisulfides) with multiple metallicconstitutions and intrinsic layered structure, which are coined as high-entropyvan der Waals materials. Millimeter-scale single crystals with homogeneouselement distribution can be efficiently acquired and easily exfoliated orintercalated in this materials category. Multifarious physical properties likesuperconductivity, magnetic ordering, metal-insulator transition and corrosionresistance have been exploited. Further research based on the concept ofhigh-entropy van der Waals materials will enrich the high-throughput design ofnew systems with intriguing properties and practical applications.

High-entropy van der Waals materials formed from mixed metal dichalcogenides, halides and phosphorus trisulfides