Selective Induction of Molecular Assembly to Tissue‐Level Anisotropy on Peptide‐Based Optoelectronic Cardiac Biointerfaces

The conduction efficiency of ions in excitable tissues and of charged species in organic conjugated materials both benefit from having ordered domains and anisotropic pathways. In this study, a photocurrent‐generating cardiac biointerface is presented, particularly for investigating the sensitivity of cardiomyocytes to geometrically comply to biomacromolecular cues differentially assembled on a conductive nanogrooved substrate. Through a polymeric surface‐templated approach, photoconductive substrates with symmetric peptide‐quaterthiophene (4T)‐peptide units assembled as 1D nanostructures on nanoimprinted polyalkylthiophene (P3HT) surface are developed. The 4T‐based peptides studied here can form 1D nanostructures on prepatterned polyalkylthiophene substrates, as directed by hydrogen bonding, aromatic interactions between 4T and P3HT, and physical confinement on the nanogrooves. It is observed that smaller 4T‐peptide units that can achieve a higher degree of assembly order within the polymeric templates serve as a more efficient driver of cardiac cytoskeletal anisotropy than merely presenting aligned ‐RGD bioadhesive epitopes on a nanotopographic surface. These results unravel some insights on how cardiomyocytes perceive submicrometer dimensionality, local molecular order, and characteristics of surface cues in their immediate environment. Overall, the work offers a cardiac patterning platform that presents the possibility of a gene modification‐free cardiac photostimulation approach while controlling the conduction directionality of the biotic and abiotic components. This work presents a cardiac photoconductive biointerface capable of inducing biomolecular assembly ordering and anisotropic cellular organization. In particular, it is demonstrated that 1D nanoassemblies comprised of π‐conjugated peptides with high degree of molecular ordering on nanogrooved polymeric templates can effectively induce cardiac cytoskeletal anisotropy and sarcomeric alignment through nanotopographic cues with potential photostimulation ability.