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A general synthesis of carbon nitride (CN) films with extended optical absorption, excellent charge separation under illumination, and outstanding performance as a photoanode in water-splitting photoelectrochemical cells is reported. To this end, we introduced a universal method to rapidly grow CN monomers directly from a hot saturated solution on various substrates. Upon calcination, a highly uniform carbon nitride layer with tuned structural and photophysical properties and in intimate contact with the substrate is obtained. Detailed photoelectrochemical and structural studies reveal good photoresponse up to 600 nm, excellent hole extraction efficiency (up to 62%) and strong adhesion of the CN layer to the substrate. The best CN photoanode demonstrates a benchmark-setting photocurrent density of 353 µA cm−2 (51% faradaic efficiency for oxygen), and external quantum yield value above 12% at 450 nm at 1.23 V versus RHE in an alkaline solution, as well as low onset potential and good stability.

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