We have demonstrated that the creation of hierarchical polysaccharide architectures can be achieved by using a fluidic liquid liquid interface as a dynamic template for the supramolecular spinning of polysaccharide nanofibers. The individual polysaccharide nanofibers were entangled to form extended network structures in the macroscopic strand, which is never produced through conventional renaturing of polysaccharide. The wrapping of a synthetic functional polymer by the polysaccharide also proceeded on the fluidic liquid interface, leading to the creation of polysaccharide strand having unique functionalities such as conductivity or fluorescence arising from the entrapped polymer.