This review comprehensively discusses the recent advances in biochar-based layered bimetallic (BC/LDHs) composites in the field of environmental pollutant removal. Firstly, the preparation methods of BC/LDHs materials, including co-precipitation, co-pyrolysis and hydrothermal synthesis, and the modulation of material properties by means of heterogeneous atom doping, chemical impregnation and fugitive magnetization enhancement are discussed in detail. Secondly, the effectiveness of BC/LDHs materials in the removal of dyes, heavy metals, nutrient salts and antibiotics was clarified, and the key mechanisms of their removal of environmental pollutants were analyzed and summarized. Further, the limitations of BC/LDHs materials in environmental applications are assessed, including the removal efficiency of specific pollutants, the adaptability under complex environmental conditions, and the long-term stability of the materials. Finally, corresponding solution strategies are proposed to address these challenges, providing new perspectives and research directions to promote the application of BC/LDHs materials in environmental pollutant removal.