these cases, most of the electrocatalysts are powdery, they should be pasted on conductive substrate (e.g., glassy carbon or carbon cloth electrode) with polymer binders (e.g., polytetrafluoroethylene or nafion); this would sacrifice part of ionsaccessible surface areas of catalysts and also bring additional contact resistances to the electrode. [12] Another popular case is to directly grow active species on the 3D nickel foams; the high porosity of nickel foams can provide active species with unblocked contact with electrolytes and can also efficiently release generated bubbles. [22] However, the intrinsic low conductivity and poor stability of nickel substrate induced unsatisfied durability of composite catalysts. Furthermore, these above mentioned catalysts, either powdery catalysts or nickel foam supported catalysts, often exhibit poor activities at low mass loadings, or exhibit high areal activities only at high mass loadings, thereby resulting in their poor mass activities and low utilizations of active species. The above disadvantages of existing catalysts invisibly increase the production costs of catalysts and reactions, which are far away from the requirements for industrialization. More efficient, costeffective, and durable catalysts/electrodes are urgently needed to promote the practical industrialization of water splitting. Herein, we introduce a versatile solution-processing method to fabricate large-scale, flexible, and conductive films directly as catalytic electrodes for water splitting. This film electrode takes bimetal components as active species, greatly improved the specific activities of prominent catalysts. It also takes graphene sheets as metal carriers and film-forming agent, facilitating the fast charge transfers and sufficient utilization of metal surfaces. The obtained graphene-bimetal film has excellent comprehensive performances with high areal activity even at a low mass loading of 0.05 mg cm −2 , and a record-high mass activity for water splitting with respect to reported works. The assembled two-electrode configuration delivers a cell voltage of 1.58 V at 10 mA cm −2 , as well as a long-term stability over 200 h; these performances are much superior to those of commercial Pt/C||IrO 2 coupled with the same mass loading and also surpass most of reported systems for the same purpose. Furthermore, this system also worked well at large sizes, and its performance can be further increased via raising the bath temperatures. Given the above superiorities, this graphene-bimetal film can be taken as a practical example to propel the industrialization of water splitting.The practical industralization of water splitting needs high-efficient and costeffective catalytic electrodes. A versatile and scalable solution-processing method to prepare such a catalytic electrode with high flexibility and conductivity is introduced. This preparation method is applicable for a wide variety of metal species and takes graphene sheets as metal carriers and filmforming agents, resulting in 100% utilization of...