The nonlinear optical properties of coumarin 343 (C343) dye-attached TiO2 nanoparticles in the size range 5-8 nm adsorbed at the interface of water/1,2-dichloroethane have been studied by using the surface second harmonic generation technique. No second harmonic (SH) response was observed from the bare TiO2 nanoparticles adsorbed at the interface, however, a strong SH response was measured from the dye molecules attached at the surfaces of the nanoparticles. The increase in the SH intensity with the increase of TiO2 nanoparticle concentration in the aqueous solution of C343 is mainly due to the pre-alignment of the dye molecules at the surfaces of nanoparticles and is partly due to the third-order polarization contribution of the nanoparticles to the observed total SH response.