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Here, we designed two promising schemes to realize the high-entropy structurein a series of quasi-two-dimensional compounds, transition metaldichalcogenides (TMDCs). In the intra-layer high-entropy plan, (HEM)X2compounds with high-entropy structure in the MX2 slabs were obtained, here HEMmeans high-entropy metals, such as TiZrNbMoTa. And superconductivity with aTc~7.4 K was found in a Mo-rich HEMX2. On the other hand, in the intercalationplan, we intercalated HEM-atoms (FeCoCrNiMn) into the gap between thesandwiched-MX2 slabs resulting in a series of (HEM)xMX2 compounds, x in therange of 0~0.5, in which HEM is mainly composed of 3d transition metalelements, such as FeCoCrNiMn. As the introduction of multi-component magneticatoms, ferromagnetic spin-glass states with strong 2D characteristics ensued.Tuning the x content, three kinds of two in the high-entropy intercalated layerwere observed including the 1*1 triangular lattice and two kinds ofsuperlattices \sqrt3*\sqrt3 and \sqrt3*2 in x=0.333 and x>0.5, respectively.Meanwhile, the spin frustration in the two-dimensional high-entropy magneticplane will be enhanced with the development of \sqrt3*\sqrt3 and will bereduced significantly when changing into the \sqrt3*2 phase. The high-entropyTMDCs and versatile two-dimensional high-entropy structures found by us possessgreat potentials to find new physics in low-dimensional high-entropy structuresand future applications.

Designation of Intra-layer and Intercalated High Entropy Quasi-2D Compounds