Ferroelectricity in Langmuir-Blodgett (LB) films (Z-type and alternated Y-type) of nitrogencrown (NC) and arachidic acid (AA) was investigated by electric polarization measurements and surface pressure-molecular area (π-A) isotherm. For Z-type AA LB multilayer and the AA LB films incorporating barium and manganese ions, as well as for Z-type NC LB multilayer and the Y-type NC/AA alternating LB films, typical hysteresis loops of the samples were observed and confirmed existence of the remnant polarizations in the LB films. Their corresponding remnant polarizations were found to be 15, 180, 650, 450 and 9400 μC·m-2, respectively. Therefore, it was demonstrated that the enhancement of ferroelectricity in the LB films could be created by incorporation of barium and manganese ions into the LB film structures and strong interaction between alternating monolayers of the samples. These novel approaches can be employed to create strong ferroelectric LB films to make ferroelectric thin-film device for practical applications.