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A series of novel calix[4]arene metal-free dyes,featuring macrocyclic structure and unique conical confor-mation,has been introduced into photoanode-based dye-sensitized electrochemical cell system as photosensitizers.The electrochemical properties of the corresponding sensitized photoanodes were systematically studied in the absence/presence of water oxidation catalyst(WOC).Furthermore,the visible-light-driven overall water-splitting reactions were conducted by fully assembled devices,obtaining a performance trend of Calix-3＞Calix-2＞Calix-1.The corresponding device of Calix-3 exhibited the best photoactivity,giving an initial photocurrent density of ca.300 μA/cm2,an IPEC peak value of ca.9.0％at 365 nm and a wide photo-respond band up to ca.620 nm.The best performance of Calix-3 can be attributed to its most effective light-harvesting ability,best ICT transition property,highest oxidation potential and thus best ability of activating WOC.This work offers an inspiration for the application of new-type effective metal-free sensitizers in photocatalytic water-splitting device.