The rapid advancement of two-dimensional (2D) materials has revolutionized materials science, offering transformative opportunities in nanoelectronics, optoelectronics, and quantum technologies. To realize the applications of 2D materials in these fields, the synthesis of high-quality, large-area, single-crystal 2D films is necessary. In the past decade, with a deep understanding of the nucleation and alignment mechanisms, the synthesis of wafer-scale single-crystal 2D materials has been realized consecutively. However, studies on wrinkle suppression, precise control of layer thickness, and stacking configurations are still at a primary stage. This perspective investigates these key factors influencing the structure and properties of 2D materials, highlighting the possible opportunities to improve their growth controllability. We believe that these insights will further enhance the controllable synthesis of 2D materials and facilitate their widespread applications.