Modulation of Metal and Insulator States in 2D Ferromagnetic VS2 by van der Waals Interaction Engineering

2D transition‐metal dichalcogenides (TMDCs) are currently the key to the development of nanoelectronics. However, TMDCs are predominantly nonmagnetic, greatly hindering the advancement of their spintronic applications. Here, an experimental realization of intrinsic magnetic ordering in a pristine TMDC lattice is reported, bringing a new class of ferromagnetic semiconductors among TMDCs. Through van der Waals (vdW) interaction engineering of 2D vanadium disulfide (VS 2 ), dual regulation of spin properties and bandgap brings about intrinsic ferromagnetism along with a small bandgap, unravelling the decisive role of vdW gaps in determining the electronic states in 2D VS 2 . An overall control of the electronic states of VS 2 is also demonstrated: bond‐enlarging triggering a metal‐to‐semiconductor electronic transition and bond‐compression inducing metallization in 2D VS 2 . The pristine VS 2 lattice thus provides a new platform for precise manipulation of both charge and spin degrees of freedom in 2D TMDCs availing spintronic applications.