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To achieve specific applications, it is always desirable to design new materials with peculiar topological properties. Herein, based on a D2h B2Cu6H6 molecule with the unique chemical bonding of planar pentacoordinate boron (ppB) as a building block, we constructed an infinite CuB monolayer by linking B2Cu6 subunits in an orthorhombic lattice. The planarity of the CuB sheet is attributed to the multicenter bonds and electron donation-back donation, as revealed by chemical bonding analysis. As a global minimum confirmed by the particle swarm optimization method, the CuB monolayer is expected to be highly stable, as indicated by its rather high cohesive energy, absence of soft phonon modes, and good resistance to high temperature, and thus is highly feasible for experimental realization. Remarkably, this CuB monolayer is metallic and predicted to be superconducting with an estimated critical temperature (Tc) of 4.6 K, and the critical temperature could be further enhanced by tensile strains (to 21 K at atmospheric pressure). 

Abstract Electrical control of atom‐thick van der Waals (vdW) ferromagnets is a key toward future magnetoelectric nanodevices; however, state‐of‐the‐art control approaches are volatile. In this work, introducing ferroelectric switching as an aided layer is demonstrated to be an effective approach toward achieving nonvolatile electrical control of 2D ferromagnets. For example, when a ferromagnetic monolayer CrI₃and ferroelectric MXene Sc₂CO₂come together into multiferroic heterostructures, CrI₃is controlled by polarized states P↑ and P↓ of Sc₂CO₂. P↑ Sc₂CO₂does not change the semiconducting nature of CrI₃, but surprisingly P↓ Sc₂CO₂makes CrI₃half‐metallic. Nonvolatility of the electrical switching between two oppositely ferroelectric polarized states, therefore, indirectly enables nonvolatile electrical control of CrI₃between ferromagnetic semiconductor and half‐metal. The heterointerface‐induced half‐metallicity in CrI₃is intrinsic without resorting to any chemical functionalization or external physical modification, which is rather beneficial to the practical application. This work paves the way for nonvolatile electrical control of 2D vdW ferromagnets and applications of CrI₃in half‐metal‐based nanospintronics.