Lead halide perovskites (APbX3) are an unusual class of ionic semiconductors that first entered the scene as efficient solar absorbers in photovoltaics, and have since been adapted into colloidal nanocrystal (NC) form. The latter emit bright light and bear unique optoelectronic properties that set them apart from their metal chalcogenide quantum dot (QD) forerunners, including a bandgap that is tailorable across the visible range by halide selection (X = Cl, Br, I), a soft, dynamic lattice that undergoes facile ion-exchange and chemical rearrangement, extremely fast photoluminescence decay rates, and an innate defect tolerance the lifts the need for epitaxial passivation to achieve high luminescence. Unlike bulk polycrystalline films, reducing the ABX3 dimensions to the nanometer scale opens a large surface area and renders them dispersible in organic media, permitting intimate mixing with organic polymer and optoelectronic components than can lead to emergent new properties. Several volumes could be dedicated alone to the study of the inorganic chemistry, morphology and photophysics of nanocrystalline perovskites; in the first part of Chapter 1, a condensed, holistic description of their crystal structure, optical properties, ion-exchange behavior, shape-control mechanisms, chemical transformations, and unconventional surface chemistry is presented. In the second half, recent progress in the area of perovskite-organic hybrid materials is interpreted against this backdrop. In the ensuing chapters, efforts to design novel perovskite-organic designer materials are described. In Chapter 2, amphiphilic, zwitterion block copolymers are synthesized and used directly in the hot injection synthesis of CsPbBr3 NCs, permitting their direct attachment to the NC surface without intermediate ligand exchange steps. In Chapter 3, polystyrene derivatives with ammonium halide pendant groups are used to tune nanocomposite color in thin films and control the kinetics of inter-NC halide exchange. In Chapter 4, precise-length, π-conjugated zwitterions are introduced as replacements for the typical aliphatic ligands used on CsPbBr3 surfaces, demonstrating the impact of doing so on energy transfer (between ligand and perovskite) and NC-packing geometry in films. In Chapter 5, the photocatalytic activity of the perovskite NC is exploited in a new photolithography process for patterning fluorescence color (and shape) into nanocomposite films. Lastly, Chapter 6 entails a discussion of the future of this field, with commentary on lead-free perovskite NC compositions.