Nanocrystals formation and fractal microstructural assessment in Au/Ge bilayer films upon annealing have been investigated by transmission electron microscopy and high-resolution transmission electron microscopy observations. Experimental results indicated that the microstructure of the metal Au film plays an important role in metal-induced crystallization for Au/Ge bilayer films upon annealing. Synchronously, the crystallization processes of amorphous Ge accompanied by the formation of Ge fractal clusters, which were composed of Ge nanocrystals. We found that the grain boundaries of polycrystalline Au film were the initial nucleation sites of Ge nanocrystals. High-resolution transmission electron microscopy observations showed successive nucleation of amorphous Ge at Au grain boundaries near fractal tips. The crystallization process was suggested to be diffusion controlled and a random successive nucleation and growth mechanism. © 2004 Elsevier B.V. All rights reserved.