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Carbides are commonly regarded as efficient hydrogen evolution reaction (HER) catalysts, but their poor oxygen evolution reaction (OER) catalytic activities seriously limit their practical application in overall water splitting. Here, vertically aligned porous cobalt tungsten carbide nanosheet embedded in N‐doped carbon matrix (Co6W6C@NC) is successfully constructed on flexible carbon cloth (CC) as an efficient bifunctional electrocatalyst for overall water splitting via a facile metal–organic framework (MOF) derived method. The synergistic effect of Co and W atoms effectively tailors the electron state of carbide, optimizing the hydrogen‐binding energy. Thus Co6W6C@NC shows an enhanced HER performance with an overpotential of 59 mV at a current density of −10 mA cm−2. Besides, Co6W6C@NC easily in situ transforms into tungsten actived cobalt oxide/hydroxide during the OER process, serving as OER active species, which provides an excellent OER activity with an overpotential of 286 mV at a current density of −10 mA cm−2. The water splitting device, by applying Co6W6C@NC as both the cathode and anode, requires a low cell voltage of 1.585 V at 10 mA cm−2 with the great stability in alkaline solution. This work provides a feasible strategy to fabricate bimetallic carbides and explores their possibility as bifunctional catalysts toward overall water splitting.

A clean N2-plasma was employed to develop self-supported porous tungsten nitride nanowires on carbon cloth (WN NW/CC) as an efficient 3D electrocatalyst for hydrogen evolution. The resulting catalyst gives a high activity and outstanding stability in both acidic and alkaline solutions.

A 3D-composite structure of FeP nanorods on vertically aligned graphene nanosheets has been fabricated for the high-performance hydrogen evolution reaction.