Thermally-responsive, short elastin-like peptides (ELPs) of sequence VPGVG (V, P and G represent valine, proline and glycine respectively), bearing different N-terminal functional groups (amino-, N-acetyl and thiol) and a non-ionisable C-terminal group, were prepared by solid phase synthesis. The conformation and aggregation properties of the ELPs were studied in different pH aqueous buffer solutions using UV-vis spectroscopy and circular dichroism (CD). The thiol-capped ELPs were used to prepare functionalized gold nanoparticles (GNPs), which were found to undergo thermally-triggered reversible aggregation at 40 °C. The peptide conformation and nanoparticle aggregation behaviour of the ELP–GNPs in aqueous solution were investigated by transmission electron microscopy (TEM), circular dichroism (CD) and UV-vis spectroscopy. It was found that the ELP–GNP conjugates were capable of reversible, thermally triggered aggregation at near-physiological temperatures (transition temperature of 40 °C at pH = 7.4), opening up applications in photothermal cancer therapy and diagnosis.