The self-assembly of peptides, specifically dipeptides, offers numerous advantages for biological applications. We describe an easy, versatile method of fabricating different types of zwitterionic Phe-Phe dipeptide structures (i.e., tubes and vesicles) through solvent-mediated assembly. The Stability of the dipeptide structures is increased by thin polymer coatings of poly(chloro-p-xylylene), a PPX film. We also investigated protein adsorption onto PPX-coated peptide tubes and vesicles by varying the thickness of the polymer film.