We describe the design and synthesis of carbazole functionalized isocyanides and the detailed investigation of their properties. Characterization by solid state NMR, CD, and IR spectroscopic techniques reveals that the polymer has a well-defined helical architecture. Surface-initiated polymerization of the isocyanide monomers onto various surfaces was carried out to give polymer brushes up to 150 nm thick. Insights into the electronic properties of the materials were obtained by Kelvin probe force microscopy (KPFM) and electroabsorption studies.