Abstract
Here we present a route for non‐covalent functionalization of carboxylated multi‐wall carbon nanotubes and graphene oxide with novel two‐dimensional peptide assemblies. We show that self‐assembled amino‐terminated biantennary and tetraantennary oligoglycine peptides (referred to as tectomers) effectively coat carboxylated multi‐walled carbon nanotubes and also strongly interact with graphene oxide due to electrostatic interactions and hydrogen bonding as the driving force, respectively. The resulting hybrids can be made into free‐standing conducting composites or applied in the form of thin, pH‐switchable bioadhesive coatings onto graphene oxide fibers. Monitoring of cell viability of pancreatic cell lines, seeded on those CNT hybrids, show that they can be used as two‐ and three‐dimensional scaffolds to tissue engineer tumour models for studying ex vivo the tumour development and response to treatment. This highly versatile method in producing pH‐responsive hybrids and coatings offers an attractive platform for a variety of biomedical applications and for the development of functional materials such as smart textiles, sensors and bioelectronic devices.