Ultra-small metal nanoclusters (< 2 nm), with distinct physical and chemical properties, have emerged as a new front in nanomaterial research. Integrating them with programmable biopolymers (e.g., nucleic acids and polypeptides) can impart new functionalities such as tunable luminescence and stimuli responsivity into this highly versatile system. Herein, I will discuss the synthesis and assembly of a monodispersed, thermal responsive gold nanocluster templated by a programmable polypeptide, i.e., elastin like polymer (ELP). ELP is composed of repeating units of a specific amino acids sequence, i.e. (VPGXG)n, where X can be any amino acid besides proline and n is the number of repeating units. The direct synthesis and controlled assembly of the thermal responsive gold nanoclusters with tailor-made ELP will be discussed in detail. These gold nanoclusters are characterized by various analytical tools including optical spectroscopy, mass spectrometry, electron microscopy, and X-ray photoelectron spectroscopy. Their thermal responsive properties are measured by dynamic light scattering at different temperatures. Significantly, we find that the ELP-templated gold nanoclusters exhibit considerably lower transition temperature than the free ELP, which makes them a promising probe for biomedical applications.