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The self-assembly of a hydrophobically modified biopolymer (chitosan) is described with particular reference to gelation of these systems. The hydrophobic modification consists of the attachment of long chain alkyl groups inserted randomly along the polysaccharide backbone. The attachment of these alkyl groups to hydrophobic surfaces or the insertion into nonpolar liquids provides a ubiquitous and versatile way to create hierarchical structures, particularly the formation of self-assembled gels. Such self-assembly can be used in a variety of new technologies relating to chromatography, lubrication and the environmental remediation of oil spills through gelation of surface layers.