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The carbon nanotube and carbon nanofibre (CNT-CNF) composite films are synthesized on different graphite substrate by low pressure and low temperature chemical vapor deposition. Scanning electron microscopy measurement and N2 adsorption experiment show that CNT-CNF composite films have network structure with optimal pore size distribution, which is beneficial to capacitive deionization. Atomic force microscopy result indicates that there is a strong correlation between the surface roughness of graphite and their thickness. Furthermore, the electrosorptive performance in salt solutions by employing as-grown CNT-CNF composite film is studied and found that the properties of the graphite substrate play a vital role in electrosorptive performance of CNT-CNF composite films by influencing their network structures.