J-aggregates of squarylium dyes in Langmuir films have been found to exhibit highly efficient and ultrafast nonlinear optical properties. We established a novel method for making Langmuir- Blodgett (LB) films of J-aggregates with a single absorption band at 784 nm. Deposition of the LB-films was carried out under excess compression of the Langmuir films at a constant speed. Coating the surface of the LB-film with a glassy poly-perfluorocarbon was found to enhance and stabilize the formation of J-aggregates. Characterization of morphology using a near-field scanning optical microscope (NSOM) showed that this LB-film has a highly ordered structure comprising 2- dimensional domains of J-aggregates. We also observed nonlinear-optical responses from this LBfilm. Ultrafast decay of absorption change (250 fs) with quite low saturation energy (3.4 μJ/cm2•pulse) was observed in femtosecond pump-probe measurements. These results suggest highly delocalization of excited states in the J-aggregates of this LB-film with the 2-dimensional mono-molecular layer structure which initially formed in the Langmuir film.