Layered hydroxides are promising supercapacitor electrode materials, but they generally exhibit poor energy storage abilities at high current densities. In article number 1301240, Pooi See Lee and co-workers report using chemical treatment to cause the Al in the Ni-Co-Al layered hydroxide sheets to be selectively etched by OH- anions, producing random defects on the Ni-Co-Al layered hydroxide sheets. Meanwhile, part of the less conducting Co2+ is oxidized into more conductive Co3+. The etched layered hydroxides show enhanced electrical conductivity and much better electrochemical performance.