The composite of VGSs/CFs (felt) was prepared by growing vertical graphene sheets on the carbon fiber felt via the chemical vapor deposition method. It can be widely used as electrodes in electrochemistry, catalyst carrier, Li/Na/S carrier, current collector in batteries/supercapacitors, composites materials with electrically conductive/thermal conductive/high strength properties, flexible conductor, or in the applications of electromagnetic shielding, sound absorption, energy storage, catalysis, adsorption and purification, etc.