The fabrication of 2D materials, such as transition metal dichalcogenides (TMDs), in geometries beyond the standard platelet‐like configuration exhibits significant challenges which severely limit the range of available morphologies. These challenges arise due to the anisotropic character of their bonding van der Waals out‐of‐plane while covalent in‐plane. Furthermore, industrial applications based on TMD nanostructures with non‐standard morphologies require full control on the size‐, morphology‐, and position on the wafer scale. Such a precise control remains an open problem of which solution would lead to the opening of novel directions in terms of optoelectronic applications. Here, a novel strategy to fabricate position‐controlled Mo/MoS2 core–shell nanopillars (NPs) is reported on. Metal‐Mo NPs are first patterned on a silicon wafer. These Mo NPs are then used as scaffolds for the synthesis of Mo/MoS2 core/shell NPs by exposing them to a rich sulfur environment. Transmission electron microscopy analysis reveals the core/shell nature of the NPs. It is demonstrated that individual Mo/MoS2 NPs exhibits significant nonlinear optical processes driven by the MoS2 shell, realizing a precise localization of the nonlinear signal. These results represent an important step towards realizing 1D TMD‐based nanostructures as building blocks of a new generation of nanophotonic devices.