Hybrid organic-inorganic materials offer a powerful platform for synergistically combining molecular tunability with collective, long-range ordered physical states. Yet achieving stable, surface addressable, and low-dimensional extended lattice hybrids—especially in true one-dimensional (1D) form—remains a key challenge. In this talk, I will describe my efforts to understand the chemistry and physics of 1D solids that manifest persistent metallic character in the bulk and how their physical states and physical properties evolve upon hybrid interfacing and co-assembly with organic functional groups. Beginning at the bulk scale, I present the vapor-phase synthesis of tellurium-rich In_2–dMo₆Te₆ single crystals with ordered indium vacancies, yielding robust anisotropic metallic transport and suppression of charge density wave behavior. Scaling down to few microns, I demonstrate a solution-phase ionic functionalization route to hybrid In_2–dMo₆Te₆ nanocrystals that retain their conductive backbone while gaining tunable solubility and optical activity. At the few nanometer scale, interfacing [Mo₆Se₆]^2– chains  with enantiopure poly-lysine produces bio-inorganic nanowires exhibiting induced circular dichroism and promising spin-elective transport. Finally, at the molecular scale, I discuss topochemical deintercalation of CaSi to isolate covalently bonded silicon chains with H/OH surface terminations, expanding main-group 1D frameworks beyond traditional chalcogenides. Taken together, these studies establish modular strategies for the deliberate design of hybrid 1D materials with tailored electronic, chiroptical, and sensing capabilities—advancing the frontier of low-dimensional functional systems.