Controlled Growth and Thickness‐Dependent Conduction‐Type Transition of 2D Ferrimagnetic Cr2S3 Semiconductors

2D magnetic materials have attracted intense attention as ideal platforms for constructing multifunctional electronic and spintronic devices. However, most of the reported 2D magnetic materials are mainly achieved by the mechanical exfoliation route. The direct synthesis of such materials is still rarely reported, especially toward thickness‐controlled synthesis down to the 2D limit. Herein, the thickness‐tunable synthesis of nanothick rhombohedral Cr2S3 flakes (from ≈1.9 nm to tens of nanometers) on a chemically inert mica substrate via a facile chemical vapor deposition route is demonstrated. This is accomplished by an accurate control of the feeding rate of the Cr precursor and the growth temperature. Furthermore, it is revealed that the conduction behavior of the nanothick Cr2S3 is variable with increasing thickness (from 2.6 to 4.8 nm and >7 nm) from p‐type to ambipolar and then to n‐type. Hereby, this work can shed light on the scalable synthesis, transport, and magnetic properties explorations of 2D magnetic materials. The thickness‐tunable synthesis of rhombohedral Cr2S3 flakes is first achieved via a facile chemical vapor deposition route by a unique design of the metal precursor and a precise control of the growth temperature. Particularly, the conduction behavior of the nanothick Cr2S3 is variable with increasing thickness, i.e., from p‐type to ambipolar, and then to n‐type.