The direct synthesis of nanostructured electrode materials on three-dimensional substrates is important for their practical application in electrochemical cells without requiring the use of organic additives or binders. In this study, we present as imple two-step process to synthesize as table core-shell structured cobaltsulfide/cobalt aluminumh ydroxide nanosheet (LDH-S) for pseudocapacitor electrode application. The cobalt aluminum layered doubleh ydroxide (CoAl-LDH) nanoplates were synthesized in basic aqueous solution with ak inetically-controlled thickness. Owing to the facile diffusion of electrolytes through the nanoplates,t hin CoAl-LDH nanoplates have higher specific capacitance values than thick nanoplates. The as-grown CoAl-LDH nanoplates weret ransformed into core-shell structured LDH-S nanosheets by as urface modification processi nN a 2 Sa queous solution.T he chemically robustc obalt sulfide (CoS) shell increased the electrochemical stability comparedt ot he sulfide-free CoAl-LDH electrodes. The LDH-S electrodes exhibited high electrochemical performance in terms of specific capacitance and rate capability with ag alvanostatic discharge of 1503 Fg À1 at acurrent density of 2Ag À1 and as pecificc apacitance of 91 %a t5 0Ag À1 .[a] Dr.