The structure and properties of Langmuir-Blodgett films of copolymers of a hydrophilic isocyanide and an isocyanide containing an NLO-active moiety with a spacer group are studied. Depending on the ratio of the two monomers, the copolymers are able to form stable monolayer films. The orientations of the NLO groups in the copolymers with respect to the film plane have been derived from polarized transmission and grazing incidence reflection (GIR) IR spectra. Quantitative analysis pf the spectra shows that the polymer main chains have no specific orientation in the plane of the film. The side chains of copolymers with a high NLO-dye content appear to be oriented perpendicular to the him plane.