In an attempt to produce polymeric pyroelectric Langmuir-Blodgett films, three derivatives of a hexadec-1-ene-maleic anhydride alternating polymer and two poly-(vinyl pyridine) derivatives have been deposited as alternate-layer films using a two-compartment trough. 1-Docosylamine and 22-tricosenoic acid were also alternated with some of the above polymers. Pyroelectric coefficients measured by the quasi-static technique were found to have a maximum value of 0.8 μC m−2 K−1, comparable to that of other Langmuir-Blodgett structures. Relative permittivity and dielectric loss values of pyroelectric films (in the range 10 Hz-100 kHz) were typically 4 and 0.06 respectively. Finally, these parameters are compared with those of commonly used pyroelectric organic materials.