Little imagination is needed to gauge the impact of lowdimensional nanostructures such as 0D quantum dots (QDs) and nanocrystals (NCs), [1][2][3][4] 1D nanowires (NWs) and nanotubes, [5,6] and 2D atomic sheets (graphene, MoS 2 , etc.). [7][8][9] With the exponential increase in the discovery of low-dimensional nanostructures, and in understanding how different and how peculiar the electrons behave when confined in the 0D, 1D, and 2D limits, an immediate next step is followed to use these low-dimensional nanostructures as "lego" pieces to build a variety of devices for electronic, photonic, and optoelectronic applications with functionality and performance unprecedented by, or better than that of, their counterparts based on conventional 3D materials. In such a quest, nanohybrids with regard to either heterostructures of the low-dimensional nanostructures, or their heterostructures with conventional materials (bulks, films, polymers, etc.), have emerged as an important class of nanomaterials for practical applications in electronic devices, photonic devices, optoelectronic devices, structural devices, medicine, sensors, etc. In fact, the past decade or so has witnessed exciting progress made in the research and development of nanohybrids, promoted particularly by the discovery of a large variety of 2D atomic materials including graphene, transition metal dichalcogenides (TMDCs), etc. [7][8][9] Despite differences in various nanohybrids stemming from different device requirements, all nanohybrids have one thing in common: the presence of heterojunction interfaces that play a critical role in the functionality and performance of the nanohybrids-based devices. This explains an intensive effort in recent research toward understanding and controlling such interfaces. Optoelectronic nanohybrids, such as QDs/graphene nanohybrids, present an excellent example. During the optoelectronic process of light absorption, exciton (or photogenerated electronhole pairs) dissociation into free charge carriers, charge transfer, and transport, the QD/graphene interface affects almost the entire process by providing the required band-edge offset for exciton dissociation and the electric field to drive the charge transfer. As the dimensions or at least one of the dimensions of the low-dimensional nanostructures approach from sub-nm to a few nm, the effect of such heterojunction interfaces on the nanohybrid properties becomes increasingly critical and controlling such interfaces must be at an atomic scale. This represents a major challenge toward achieving the anticipated nanohybrids' device performance, especially in practical applications that require wafer-scale synthesis, manipulation, and characterization of these atomically small, single-crystalline lowdimensional nanostructures. It should be noted that many excellent reviews or book chapters are available in literature covering the recent progress made in fabrication, characterization, and applications of nanohybrids. [8][9][10][11][12][13][14][15][16] Instead, this article intend...