We report for the first time the enhanced capacitance of multi-walled carbon nanotubes (MWCNTs) after exfoliation. Transmission electron microscopy studies confirmed that the MWCNTs were partially exfoliated with improved effective surface area. Carbon cloth electrode deposited with partially exfoliated carbon nanotubes (Ex-CNTs) yielded specific capacitances in a range of 130–165Fg−1 at charging/discharging current densities from 5 to 0.5Ag−1, with coulombic efficiencies of ∼98%. The specific capacitance of Ex-CNTs was an order of magnitude higher than untreated MWCNTs, and comparable to graphene at all charging/discharging current densities we studied. The enhanced capacitance can be attributed to improved effective surface area and increased defect density of the exfoliated tubular structure. The results declared that Ex-CNTs are promising electrode materials for high-capacitance supercapacitors.