NiFe layered double hydroxides (NiFe LDHs) have been intensively developed for the oxygen evolution reaction (OER) in alkaline media; however, their unsatisfactory hydrogen evolution reaction (HER) performance limits their practical application in overall water splitting. Herein, a simple and efficient one-step electrodeposition method is used to accomplish in situ growth of NiFe LDHsNiFe alloy gradient hybrid coatings on a carbon cloth (CC). Within the binder-free electrode, NiFe LDHs nanosheets with a low-crystalline nature exhibit highly active bifunctional OER/HER activities, and the NiFe ...