Amorphous C:S:N:H thin-film materials were produced from methyl, propyl-, allyl-, and phenyl isothiocyanate source compounds in plasma chemical vapor deposition (PCVD). The PCVD process was investigated in terms of the deposition yield and pressure increase in the reactor. These parameters provide insight into the mechanism of plasma activation of the organoisothiocyanates. The films are characterized in terms of their structure, elemental composition, optical absorption and electrical conductivity. The ultraviolet-visible (UV-VIS) spectral data account for the presence of two optical gaps in the examined materials. The light absorption is related to the excitation of electrons with a contribution by the localized states of molecular nature, which contain pi-bonds. The materials, owing to their rather low conductivities (not exceeding 10(-11) S m(-1)), can be classified as dielectrics. The thermal treatment of the films in nitrogen was found to increase the conductivity by three orders of magnitude. The films reveal a substantial photoconductivity effect which appears to be sensitive to the light wavelength. The evaluated quantum yield values are 10(-5)-10(-4) el. quant(-1).