Temperature-triggered formation of nanostructures with distinct biological activity offers opportunities in selective modification of matrices and in drug delivery. Toward these ends, diblock polymers comprising poly(diethylene glycol methyl ether methacrylate) (PDEGMEMA) conjugated to a triple helix-forming collagen-like peptide were produced. Triggered by the collapse of the thermoresponsive domain above its LCST, the conjugate undergoes a reversible transition in aqueous solution to form well-defined nano-vesicles with diameters of approximately 100 nm, with a transition temperature of 37°C. The incorporation of CLP domains in these nano-structures may offer opportunities for the selective targeting of collagen-containing matrices.