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Second harmonic generation (SHG) in the oriented film of symmetric squaraine (Sq) was studied. Oriented Sq film on aligned polytetrafluoroethylyne (PTFE) sublayer prepared by vacuum deposition with subsequent rubbing using a cloth has been obtained. However, the mechanisms of orientation and SHG are still not clear. Methyl and ethyl substituted hydroxyl-Sq (OHSq) compounds formed oriented films with dichroic ratio of 8 on PTFE layer but with dichroic ratio of 1,5 on Teflon AF. Second layer deposition of Me-OHSq on Et-OHSq or of Et-OHSq on Me-OHSq led to an increase of the film dichroic ratio. Only the film, where Me-OHSq was first layer, exhibits an increase of SHG signal after deposition of second layer. Small differences in bi-layered OHSq films structure was detected by X-Ray diffraction (XRD) spectra.