Peptide-Functionalized Nanopillared Surfaces with Tunable Antimicrobial and Immunomodulatory Properties

Stimuli-responsive nanopatterned surfaces developed by physical and chemical modification with polymers, nanoparticles, and biomolecules have found various applications in biotechnology and biomedicines. In this study, bacterial capture and killing abilities of cicada wing-inspired, highly hydrophilic, nanopillared surfaces composed of poly-(methacrylic acid)-<i>co</i>-poly-(vinyl alcohol) are combined with cationic amphipathic peptides to develop antimicrobial and immunomodulatory materials with tunable properties. The peptide-modified surfaces prepared by layer-by-layer deposition were analyzed for the amount of peptide deposited and demonstrated significant changes in surface hydrophilicity and height of nanopillars upon biomolecule immobilization. The deposition of an antimicrobial peptide on nanopillared surfaces reduced the antimicrobial properties of the bare surfaces and the free peptide, while the immobilized peptide activated Toll-like receptors of macrophages, thereby enhancing the immunomodulatory properties of the materials. The gradual degradation of peptides on the modified surfaces in biological milieu slowly dampened immunomodulatory properties and restored the antimicrobial efficacies of the bare surfaces as a function of time, suggesting the development of tunable and regenerative materials with potential applications in wound healing.