Stimuli-responsive materials are playing an increasingly important role in a wide range of applications such as drug delivery, diagnostics, sensors, and tissue engineering. Among them, gold nanoparticles responding to changes in their surrounding environment are of particular interest due to their size-related optical properties. Here, we present a novel strategy for the preparation of gold nanoparticles exhibiting a stimuli-responsive behavior. We rely on the use of a ligand consisting of only a single repeat of the elastin-based pentapeptide VPGVG. In this contribution, we describe a protocol for the solid-phase peptide synthesis of thiol-terminated VPGVG ligand, and for the preparation of gold nanoparticles covered with the pentapeptide through a ligand-exchange reaction.