A new class of carbosiloxane dendrimer (G4-48PyP) terminated with 4-pyridylpropano I was synthesized and its possible application to functional thin films was examined through metal complexation and Langmuir-Blodgett (LB) technique. The highly concentrated periphery pyridyl groups of G4-48PyP were exposed on aq. aluminum ions at the air-water interface. The monolayers showed stability up to ca. 50 mN/m of surface pressure. When the subphase became acidic or alkaline, the monolayers changed to condensed phase. The presence of aluminum ions also caused reduction of the molecular area. The macroscopic images of the monolayers were monitored by Brewster angle microscopy (BAM) and only the images of dendrimer aggregates could be observed after the monolayer collapse. The surface images of the monolayer LB film were scanned by atomic force microscopy (AFM). The convex structures of single and aggregate molecules were directly observed. The structures of Langmuir-Blodgett (LB) films were characterized by FT-IR, UV-Vis, and X-ray photoelectron spectroscopy (XPS). The UV-Vis spectrum of the aluminum ion-complexed LB film showed additional band around 670nm, which was not found in the spectra of dendrimer itself or aq. aluminum ions. XPS spectra also supported the incorporation of aluminum ions into the LB films.