Beyond Monolayers: Opportunities and Challenges in Wafer‐Scale Multilayer Transition Metal Dichalcogenides

Multilayer transition metal dichalcogenides (TMDs), with their tunable layer numbers and stacking configurations, provide a key platform for designing electronic and optical properties beyond the monolayer limit, promising to drive the development of next‐generation semiconductor technologies. However, the promise of multilayer TMDs remains limited by the lack of scalable synthesis routes that enable large‐area growth with precise control over thickness, stacking sequence, and material quality. From the perspective of energy competition during the growth process, we systematically analyze four principal growth paradigms: layer‐by‐layer epitaxy, step‐edge‐guided‐growth, hypotaxy (‘hypo’ meaning downward and ‘taxy’ meaning arrangement), and interfacial epitaxy, while also outlining corresponding improvement strategies for each paradigm. Looking forward, we discuss the future trajectory of the field, highlighting the viable routes to evolve from the current paradigm of imprecise kinetic control to one of atomically precise fabrication. This perspective not only furnishes tangible strategies but also provides promising directions for achieving the controlled, scalable production of large‐area multilayer TMDs.