Lignocellulose nanofibrils (LCNFs), as an emerging member of the green nanofibril family, have tremendous potential in improving the dispersibility, adsorption and photogenerated carrier separation efficiency of BiOBr because of the combination of the advantages of nanocellulose (NC) and nanolignins. Herein, sulfated lignocellulose nanofibrils (SLCNFs) were obtained from the poplar alkaline peroxide mechanical pulp (APMP) using a deep eutectic solvent (DES) and a mechanical defibrillation strategy, and flower-like BiOBr/SLCNF composites with oxygen vacancies were prepared by in situ synthesis. Due to the well-preserved lignin structure, abundant oxygen-containing functional groups, and the interconnected three-dimensional mesh structure in SLCNFs, the composites exhibited flower-like morphology, good dispersion and excellent adsorption performance after the introduction of SLCNFs. EPR analysis showed that the introduction of SLCNFs increased the number of oxygen vacancies in BiOBr, which improved the visible light absorption and reduced the recombination of photogenerated carriers. In addition, the photocatalytic activity improved with interfacial interaction between BiOBr and SLCNFs promoting the separation of electrons and holes. Therefore, BiOBr/SLCNF can effectively remove RhB in the dynamic continuous process of adsorption enrichment and photocatalytic oxidation. Under visible light, 99% of RhB was degraded within 30 min and 88.5% of tetracycline hydrochloride (TCH) was degraded within 60 min. Importantly, the main active species which removed RhB by BiOBr/SLCNF were ˙O²⁻ and h⁺, and the BiOBr/SLCNF composites still have good stability and recyclability after 5 times of repeated use. Overall, the BiOBr/SLCNF composite photocatalyst has great potential for the purification of organic wastewater.