Pyroelectric properties in alternating DAEP/NC Langmuir-Blodgett (LB) films and effects of incorporating the barium cations on pyroelectric behaviours have been investigated.The pyroelectric coefficient measured is found to be 58μCm-2K-1 at 300K.The dielectric properties have been measured and used to determine the figures of merit in thermal devices. Relative permittivity εr and dielectric loss values tanδ of pyroelectric films (in the range of 1kHz—100kHz) are 2.34—1.96 and 0.08—0.04, respectively. The effects of different deposition and incorporated metal ions on pyroelectric properties are also discussed in this paper. It is indicated that the alternating LB films is promising in the field of pyroelectricity and pyroelectric infrared detector.