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Red phosphorus (RP) is an emerging visible‐light‐responsive photocatalyst, yet the rapid charge recombination has limited photocatalytic hydrogen production activity. In this work, a Z‐scheme heterostructure with RP nanolayer coated on high‐index (116) faceted anatase TiO2 nanoparticles (TiO2@RP) is designed and fabricated via chemical vapor deposition. Compared with pristine TiO2 and RP, the optimized TiO2@RP Z‐scheme heterostructure exhibits a significantly boosted photocatalytic activity for pure water splitting, with hydrogen evolution rate reaching 12.9 µmol·h−1, under simulated solar light irradiation. The strong interfacial interaction and staggered band alignment between (116) faceted TiO2 and RP result in the formation of built‐in electric field, which can drive the directional charge migration from the conduction band (CB) of TiO2 to the valance band (VB) of RP under light irradiation, with photoelectrons and holes of high redox ability maintained at the CB of RP and the VB of TiO2, respectively. This well‐designed heterostructure greatly promotes photogenerated charge separation and migration via a direct Z‐scheme charge transfer pathway. [ABSTRACT FROM AUTHOR]

• Phosphorus-doped TiO 2 nanotube arrays (TNTAs/P) was synthesized by calcination red phosphorus with TNTAs in sealed ampoule. • TNTAs/P exhibits enhanced photoelectrocatalytic tylosin removal activity. • P dopants could improve light absorption and charge separation in TNTAs. • •OH radicals and holes are the dominant reactive species for tylosin degradation. Photoelectrocatalytic (PEC) degradation of antibiotics residues is one of the most effective strategies for wastewater treatment. TiO 2 has been widely used as an efficient photoelectrode material for pollutant removal. However, the degradation efficiency of UV light-driven TiO 2 -based photoelectrodes is still low. In this study, phosphorus-doped TiO 2 nanotube arrays (TNTAs/P) were fabricated by calcination TNTAs with amorphous red phosphorus in sealed ampoules. By tuning the amount of P dopants, the optimized TNTAs/P(0.75) photoelectrode exhibits excellent PEC degradation performance under the Xenon lamp (100 mW/cm2, λ > 300 nm) light irradiation, with 79 % tylosin removal within 250 min.. The TNTAs/P(0.75) photoelectrode also displays about 4-fold photocurrent enhancement than bare TNTAs. It is suggested that the P-doping treatment could improve the light-harvesting ability and accelerate the separation efficiency of photo-induced electron-hole pairs in TNTAs, which benefits the production of •OH radicals and thus leads to the enhancement in tylosin degradation activity. This present work demonstrates a facile approach for improving the PEC degradation efficiency by doping heteroatoms in the photoelectrode. Capsule: P-doped TiO 2 nanotube arrays were fabricated for boosting photoelectrocatalytic tylosin degradation activity due to the enhanced light absorption and charge transfer efficiency. [ABSTRACT FROM AUTHOR]