We demonstrated full determination of second-order nonlinear susceptibility of a 4′-n-octyl-4-cyanobiphenyl (8CB) liquid crystal (LC) monolayer adsorbed on a second-harmonic (SH) active polyimide (PI) substrate. In order to separate the SH signal of the LC film from that of the PI film, we adopted an interferometry technique of second-harmonic generation (SHG) using an ultra-thin film local oscillator. We have found a variety of phases in the components of susceptibility: those of χ
z
i
i
and χ
i
z
i
are almost the same but the phase of χ
z
z
z
differs by 80° from the other two. The phases of the components of the surface susceptibility tensor are not always identical. This fact indicates that the surface SH response is more complicated than what we expected.
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