Cholesterol-appended gelator 1 describing the linking of 2hydroxy-1-naphthaldehyde with cholesterol coupled benzaldehyde via hydrazine linker has been synthesized and established as multi responsive material. It forms stable gels from semiaqueous and benzenoid solvents, as well as in hydrocarbons and fuel oils. Aggregation of the gelator takes place because of the function of several weak forces in solution. Extensive π-π stacking between the naphthalene units and hydrophobic interaction exerted by the cholesterol surface encourage gelation. The phenolic À OH serves as an anion binding site. Importantly, 1,4-dioxane-H 2 O gel of 1 is CN À-responsive and shows gel-to-sol phase transformation with color and fluorescence changes selectively in presence of CN-ion. Gelator 1 also exhibits phase-selective gelation (PSG) behaviour and forms stable gels with water-immiscible solvents from their aqueous biphasic mixtures. Such phase-selective gelation of 1 avails some potential and promising real-life applicability in environmental remediation (oil spill recovery and purification of dye-contaminated water). The gel phase selectively removes cationic dyes such as Crystal Violet (CV) and Malachite Green (MG) from aqueous solution in a short time with high efficiency (∼ 99 %).