We prepared submonolayers, monolayers, and multilayers of organosiloxanes derived from the second to fourth generation (G2-G4) SiCl3-terminated carbosilane dendrons on mica by spin-casting. The surface properties of these films, such as wettabilities, surface tensions, works of adhesion with various liquids, pore size, and surface coverage, were investigated by means of contact-angle measurements. All G2-G4 films exhibit high hysteresis of similar to20degrees, probably due to molecular scale chemical heterogeneity and surface roughness. The surface tensions of the G2-G4 monolayers are similar: gammas (total) = similar to29 mJ/m(2), gammas(d) (dispersive) = similar to24 mJ/m(2), and gammas(p) (polar) = similar to5 mJ/m(2). However, only gammas(d) (similar to21 mJ/m(2)) contributes to the surface tensions of the multilayers, suggesting that the underlying polar mica substrate is significantly screened by the dendron multilayers. Works of adhesion (W-SL) for water, glycerol, dimethylformamide, methylene iodide, squalane, and hexadecane on the films were measured. The multilayers exhibit a lower W-SL(d) (dispersive) than the monolayers (difference of similar to3 mJ/m(2)), consistent with a decrease of gamma(S)(d) from monolayers to multilayers. Furthermore, both the average pore size and the surface coverage of the G2-G4 monolayers were estimated to be 0.31-1.1 nm(2) and -77%, respectively.