In this study, pyrrole monomer is polymerized on carbon nanofibres (CNFs) via electropolymerization. This is a new technique to produce a chemically bonded CNF-polypyrrole composite. Deposition of the polypyrrole (PPy) on the nanofibres was optimized by varying the degree of deposition and deposition speed. Optimization studies have proven that the high deposition amounts result in blocks of polymers, which can be overcome through tuning the degree of polymerization by means number of cycles of electropolymerization and the scan rate of the electropolymerization.