A continuous cobalt-based layered double hydroxide (LDH) nanosheet thin-film electrode has been fabricated by drying a nearly transparent colloidal solution of cobalt-based LDH nanosheets on an indium tin oxide (ITO)-coated glass plate substrate. The effects of varying the Al content, the film thickness, and the heating temperature on the electrochemical properties of the as-deposited thin-film electrode have been investigated. A thin-film electrode with a Co/Al molar ratio of 3:1, which has a large specific capacitance of 2500Fcm−3 (833Fg−1) and a good high-rate capability, shows the best performance when used as an electrode in thin-film supercapacitors (TFSCs). As the thickness of the thin film was increased from 100 to 500nm, the specific capacitance of the thin-film electrode remained essentially unchanged, which is due to the porous microstructure generated in the original electrochemical process and the low internal resistance of the thin-film electrode. The specific capacitance of the thin-film electrode showed no observable change after heating at 160°C, but decreased on further heating to 200°C, indicating that the electrochemically active Co sites inside the thin-film nanosheet electrode are already essentially fully exposed in the as-prepared material and hence cannot be further exposed through heating. Such a thin-film electrode made up of nanosheets may be a potential economical alternative electrode for use in TFSCs.