Chalcogenide glasses as nanoscale thin films have become leading candidates for several optical and photonic technologies, ranging from reflective displays and filters to photonic memories. Current material systems, however, show strong optical absorption which limits their performance efficiencies and complicates device level integration. Herein, we report sputter deposited thin films of GeSe3, which are low loss and in which the flexible nature of the atomic structure results in thermally activated tunability in the refractive index as well as in the film's physical volume. Such changes, which occur beyond a threshold temperature are observed to be accumulative and directed toward a more equilibrium amorphous state of the film, instead of crystallization. Our results provide insight into a new type of configurability that is based on strong coupling in the material's opto-structural properties. The low optical losses in this material system combined with the tunability in the optical properties in the visible and near-infrared have direct application in higher performing optical coatings and in corrective optics.