The overarching goal of this work is to explore a new method for strong direct magnetoelectric ME coupling by creating acentric building blocks of spin-orbit-entangled states and incorporate them into ME nanostructuresdevices. To test the feasibility of this approach, the focus of the supported one-year period is to address the question of how to design, synthesize and characterize the 2D ME structural unit. This question is the first step toward the ultimate goal of utilizing this 2D ME building block. The results of our first-principles calculations support the hypothesis of the proposed work that confining a 2D layer of strongly spin-orbit-coupled magnetic 5d elements in an interfacial environment would lead to ME effects larger than the conventional type-I multiferroics. A reliable computational procedure was established and applied to the prototype structure. The designed superstructures were synthesized and characterized. The key ingredients for the ME coupling were all implemented.