Thin films of multiwalled carbon nanotubes (MWCNT), graphene and polypyrrole (PPy) nanofibers were prepared by cathodic electrophoretic deposition (EPD) from aqueous suspensions, containing safranin (SAF) as a new dispersant. The results of Fourier transform infrared spectroscopy, UV-Vis spectroscopy studies and sedimentation tests, coupled with deposition yield and electron microscopy data showed that SAF adsorbed on MWCNT, graphene and PPy, provided their dispersion and charging in the suspensions and allowed efficient EPD. The deposition yield can be controlled by the variation of SAF concentration in the suspensions and deposition time. The use of SAF as a co-dispersant for MWCNT, graphene and PPy, allowed controlled EPD of composite graphene-MWCNT and graphene-PPy films. The proposed approach for the deposition of PPy paves the way for EPD of neutral polymers using organic dyes as dispersing and charging agents. The composite films were investigated for application in electrochemical supercapacitors (ES). The graphene-MWCNT and graphene-PPy films showed significant increase in capacitance, decrease in resistance and increase in capacitance retention at high charge-discharge rates compared to the films of individual components. The analysis of electrochemical testing results and electron microscopy data provided an insight into the influence of composite microstructure on electrochemical performance. The composites, prepared by EPD are promising materials for electrodes of ES. (C) 2013 Elsevier Inc. All rights reserved.