This paper reports the anisotropic electrical properties of a layer-by-layer (LBL) film composed of water-soluble conjugated polymers and single-walled carbon nanotubes (SWNTs). The water-soluble poly (p-phenylene ethynylene)s (PPEs) are capable of a strong pi-pi interaction with the sidewall of SWNTs and results in a very stable PPE-SO3/SWNTs composite in aqueous solution. Aligned LBL films were prepared by self-assembly using the anionic PPE/SWNTs and cationic PPE on various substrates. The polarized Raman spectra exhibited the cos(2)alpha polarization dependence of the G-band intensity between the polarization direction and the SWNTs alignment direction. The electric conductivity within the films can be controlled by the deposition direction in the LBL formation.