We investigated the syntheses of hybrid soft materials composed of carbon fibers and conductive polymers including nanocarbon materials, such as carbon nanotube. The surface grafting of polypyrrole onto the carbon nanotube was examined in order to obtain the highly dispersive carbon nanotube into polypyrrole matrix. The graft polymerization of pyrrole was successfully initiated by chemical oxidative polymerization in the presence of carbon nanotube having carboxyl groups on the surface. The hybrid soft materials were prepared by electrochemical polymerization of pyrrole in the presence of polypyrrole-grafted carbon nanotube, sodium dodecylbenzenesulfonate as a dispersant and an anion dopant, and carbon fiber as an electrode. The prepared hybrid soft materials revealed good electroconductivity (3.9 S/cm), which was higher than that of conductive polypyrrole alone. Furthermore, these hybrid soft materials showed formal alterations (bending, stretching and rotating) corresponding to the electric field, namely, showed electro-responsive actuation behavior.