Magnetoelectricity, the generation of magnetic moments by electric fields and vice versa, is a phenomenon discovered more than a century ago. It has gained renewed recent interests because of the discovery of new magnetoelectric materials, the notion of band topology effects in magnetoelectricity and its promise for electrical control of magnetism. In this talk, I will discuss our recent efforts in exploring magnetoelectricity in time- and inversion-asymmetric 2D materials. Two very different classes of materials, non-magnetic transition metal dichalcogenides and magnetic transition metal trihalides, will be discussed. While the former exhibits a unique orbital magnetoelectric effect originated from electronic Berry curvature effects, a large magnetoelectric effect in the latter allows robust electrical switching of its magnetic orders. Implications on electrically controlled nonvolatile memory devices will also be discussed.