Lead sulfide nanocrystals with well-defined structure and orientation were obtained on ultrathin polydiacetylene (PDA) substrates, forming a unique hybrid functional material comprised of linear arrays of size-quantized semiconductor nanocrystals that are connected via conjugated polymer strand nanowires. The deposition was carried out at the liquid-gas interface by reacting aqueous solutions of PbCl2 with controlled amounts of H2S gas. Following nanocrystal deposition, the samples were transferred onto solid substrates using the Langmuir-Schaffer technique and characterized by atomic force microscopy (AFM), transmission electron microscopy (TEM), and electron diffraction. AFM showed that the Pb2+ concentration is the main parameter that affects the growth. TEM and electron diffraction indicated that the nanocrystals are aligned with the linear PDA film, with a uniaxial orientation relationship in which the <110>PbS direction is parallel to the linear direction of the polymer substrate.