Controlling inorganic structure and dimensionality through structure directing agents is a versatile approach for new materials synthesis that has been used extensively for metal-organic frameworks and coordination polymers. However, the lack of solid inorganic cores requires charge transport through single-atom chains and/or organic groups, limiting their electronic properties. Here, we report that strongly-interacting diamondoid structure directing agents guide the growth of hybrid metal-organic chalcogenide nanowires with solid inorganic cores having three-atom cross sections, representing the smallest possible nanowires. The strong van der Waals attraction between diamondoids overcomes steric repulsion leading to a cis configuration at the active growth front, enabling face-on addition of precursors for nanowire elongation. These nanowires have band-like electronic properties, low effective carrier masses (close to one electron rest mass), and three orders-of-magnitude conductivity modulation by hole doping. This discovery highlights a previously unexplored regime of structure directing agents compared with traditional surfactant, block copolymer or metal-organic framework li nkers. Show Partial Abstract