Self‐assembled peptide microtubes are fabricated with the biopolymer chitosan. The microtubes are covalently attached to chitosan and the morphology of the chitosan assembled on the surface of the microtubes can be tuned by altering the pH of the growth solution. Cytotoxicity studies in the presence of mouse embryonic fibroblasts indicate that the chitosan‐bound microtubes are highly biocompatible and the cells are able to survive and proliferate at a similar rate to the control. Antibacterial studies in the presence of E. coli prove that the chitosan‐bound microtubes are bactericidal. This simple method for the development of biocompatible microstructures will facilitate cell targeting, fabrication of efficient carrier devices, and the preparation of highly efficient antibacterial materials.
