Low cost and large scale carbon nanotube and nanofibre (CNT-CNF) composite films have been fabricated and employed as electrodes for electrosorption of cupric ions. The regeneration of the saturated CNT-CNF film electrode has been investigated. Three methods (short-circuiting, short-circuiting and then reversing voltage, reversing voltage and then short-circuiting) are used for regeneration. The results show that low regeneration efficiency of CNT-CNF film electrode due to electrodeposition of Cu on the electrode surface can be highly improved by regeneration applying reverse voltage combined with short circuit. 93% regeneration efficiency can be achieved when 0.8 V reverse voltage is applied before short-circuiting during regeneration of CNT-CNF film electrode.