Improving the properties of the existing two-dimensional (2D) materials is a major concern for many researchers today. Synergistic coupling of single-phase 2D material species with secondary functional materials has resulted in 2D nanohybrids with significantly enhanced properties beyond the sum of their individual components. In particular, nanohybrids created by alternatingly integrating different material species in the confined 2D nanometer regime have the potential to meet the needs of a wide variety of applications, particularly the many important energy-related applications that are of interest. However, scaling up production of 2D nanohybrids is still challenging, which is a major barrier to their practical application. Delamination and exfoliation by physical means separate the weakly bound 2D nanosheets into kinetically stable single- or few-layers. Herein, we provide a concise overview of recent achievements in the physical exfoliation-based fabrication of 2D nanohybrids featuring controlled heterolayered structures. Several strategies to efficiently produce heterolayered 2D nanohybrids in large quantities are described, such as (i) coexfoliation of different 2D species, (ii) aqueous-phase synthesis, and (iii) gas-phase synthesis. The versatility of the 2D nanohybrids was also illustrated by remarkable research examples, especially in energy-related applications.