A series of structural complementary decapeptides with phenyl boronic acid tails or borono-decapeptides (BPs) were designed and synthesized for supramolecular self-assembly. After dissolving these borono-decapeptides in deionized (DI) water, well-defined nanofibers were formed in BP1 (B(OH)(2)VEKELVKEKL-OH) and BP3 (B(OH)(2)AELELARARL-OH). It was found that the self-assembled borono-decapeptide BP1 and BP3 have a parallel beta-sheet conformation in the formed nanofibers. The strategy demonstrated here shows a great prospect in preparation of well-ordered nanofibers via rationally designing the molecular structures of peptides.