Three-dimensional network of cobalt and aluminum layered double hydroxide (LDH) nanosheets was synthesized on nickel foam by a simple hydrothermal method. The CoAl-LDH nonosheets were subsequently coated by ion sputtering with thin layers of Pt films to facilitate fast electron transport between current collector and the CoAl-LDH active materials. The optimal thickness of the Pt film acquiring the best performance was identified by applying various sputtering time in controlled experiments. The supercapacitor built by the CoAl-LDH nanosheets coated with Pt film sputtered for 5min has a high specific capacitance (734.4Fg−1 at 3Ag−1), excellent rate capability as well as cycling stability. Moreover, it showed a long life of 77% retention after 6000 cycles and its general morphology was preserved after the test. The synergetic affect of conductive layer of Pt films and CoAl-LDH on the improvement of electrochemical properties was discussed and this would provide a useful clue in designing novel and effective electrode materials for supercapacitors.