Oil spill remediation remains a major challenge in global marine pollution control. Given their rapid oil removal capability, reusability, and environmental compatibility, phase-selective organogelators (PSOGs) have become attractive candidates. Nevertheless, few powdered PSOGs have been reported to rapidly form phase-selective gels with crude oils. In this work, we synthesized a series of lysine-derived organogelators (Lys-OUAs) through a simple route and evaluated their gelation behavior. In particular, Lys-OUA-C14 showed superior gelation ability and formed stable gels with a wide range of petroleum hydrocarbons. Results obtained from Fourier-transform infrared spectroscopy, UV-vis absorption spectroscopy, scanning electron microscopy, concentration-dependent and temperature-dependent 1H NMR, differential scanning calorimetry, and X-ray diffraction indicated that van der Waals forces, hydrogen bonding, and π-π stacking interactions were involved in the self-assembly of Lys-OUA-C14. Notably, Lys-OUA-C14 rapidly solidified diesel and enabled efficient recovery within 120 s through three-dimensional networks, without the need for external heating/cooling cycles or co-solvents. Powdered Lys-OUA-C14 can be readily synthesized in high yield and exhibits good oil removal efficiency, outstanding recyclability, and eco-friendliness, making it a promising material for large-scale remediation of oil-spill-contaminated water.
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