The growth of sputter-deposited Cr thin films on amorphous SiO2 during the early stages was studied using transmission electron microscopy. Amorphous three-dimensional islands were first formed, and then they grew with continuously increasing density and slowly increasing size as the deposition proceeded. When these islands began to coalesce at a nominal film thickness of 2.3–3.0 nm, they abruptly crystallized into randomly oriented crystalline nuclei. The depth profile analysis by x-ray photoelectron spectroscopy indicates the existence of interfacial Cr–O interactions. After excluding the possibilities of kinetic limitation and interfacial mixing, a thermodynamic model was employed to explain the size-dependent amorphous-to-crystalline transition. Our results suggest that the interfacial-interaction-induced strain relaxation at island/substrate interfaces might result in the thermodynamic stabilization of substrate-supported amorphous islands below a critical size. © 2003 American Institute of Physics.