<p>Biosurfactants have long been studied within the context of bioremediation due to their biological origin, low toxicity, and ability to enhance pollutant mobilization and uptake. More recently, they have also been explored as green adsorbents for pollutant removal; however, their systematic integration with clay minerals into composite adsorption systems remains comparatively underexplored. Biosurfactant–clay hybrids offer a unique opportunity to bridge bioremediation principles with engineered adsorption platforms by combining biological functionality with the structural stability and tunable interlayer architecture of clays. This review examines recent advances in biosurfactant–clay systems for the removal of heavy metal ions and organic micropollutants from water and soil matrices, with emphasis on structure–mechanism–performance relationships relevant to sustainable and circular process design. Biosurfactant intercalation modifies clay interlayer spacing, polarity, and stability, creating chemically heterogeneous environments that enable multisite adsorption through cooperative electrostatic attraction, hydrophobic partitioning, hydrogen bonding, and coordination interactions. Within this framework, heavy metal ions are predominantly captured through coordination-dominated pathways that support selective uptake and recovery, whereas organic micropollutants are mainly sequestered through partition-driven mechanisms that favor reversible adsorption. The review further examines how pollutant-class–specific mechanisms translate across water treatment and soil remediation contexts, and discusses key challenges related to intercalation stability, biosurfactant variability, scalability, and life-cycle performance. By positioning biosurfactant–clay composites within a unified structure–mechanism–performance and circular design perspective, this work highlights their potential as emerging platforms for sustainable and recovery-oriented environmental remediation.</p> Graphical Abstract <p></p>