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Well-designed hierarchical F-BiVO 4 @NiFe-LDH photoanode with a core-shell heterostructure has been successfully fabricated by F− ions etching and in situ electrochemical synthesis of NiFe-LDH onto BiVO 4 film, which demonstrates enhanced photoelectrochemical water splitting and degrada antibiotic tetracycline hydrochloride. • F-BiVO4@NiFe-LDH photoanode has been successfully developed by surface/interface engineering. • The photoanode exhibits efficient performance in PEC water splitting coupled with degradation of organic pollutants. • Experimental studies and DFT calculation reveal a synergistic effect of F doping and NiFe-LDH cocatalyst. • This strategy can be extended to other photoelectrodes for solar energy conversion and wastewater treatment. Antibiotic resistance has become a global problem as indicated by the worldwide emergence of multidrug-resistant bacteria, which makes it an urgent demand to develop effective technologies for antibiotics removal from pharmaceutical wastewater. In this work, simultaneously removing antibiotic tetracycline from wastewater coupled with pure H 2 generation has been successfully achieved through PEC technique by using F-doped BiVO 4 @NiFe-LDH (F-BiVO 4 @NiFe-LDH) core-shell photoanode. The maximum photocurrent density of the F-BiVO 4 @NiFe-LDH photoanode at 1.23 V vs. RHE is about 6-fold that of the pristine BiVO 4 photoelectrode. Furthermore, the composite photoanode was effectively applied to the PEC degradation of tetracycline hydrochloride (TCH), superior to the reported results. An experimental-computational combination study reveals that the synergistic effect between F doping and NiFe-LDH simultaneously improves the light absorption, charge separation and charge injection efficiency of BiVO 4. This work presents a sunlight-driven, efficient and sustainable method for water splitting to produce hydrogen and new insights into wastewater treatment. [ABSTRACT FROM AUTHOR]