Self-assembly of a nucleotide bolaamphiphile, terminated with two nucleotide moieties including thymine, deoxyribose, and phosphodiester at both ends of the C20 oligomethylene chain, in sodium chloride aqueous solutions has been studied by SEM, LSM, FE-SEM, micro-FTIR, and zeta-potential measurement. The self-assembly behavior of the nucleotide bolaamphiphile was strongly dependent on the concentration of sodium chloride added. The nucleotide bolaamphiphile was found to hierarchically self-assemble to form micrometer-sized fibers (microfibers) consisting of bundles of entangled nanometer-sized fibers (nanofibers) under certain conditions of sodium chloride concentration (similar to44 mM). The zeta-potential measurement suggested that the surface-charge tuning of the.nanofibers induce the hierarchical self-assembly of the microfibers. (C) 2004 Elsevier Inc. All rights reserved.