Nanostructured noble metals are of great interest because of their tunable optical and electronic properties. However, the green synthesis of anisotropic nanostructures with a defined geometry by the systematic nanoassembly of particles into specific shape, size, and crystallographic facets still faces major challenges. The present work aimed to establish an environmentally friendly methodology for synthesizing gold-based anisotropic nanostructures using starch-capped bimetallic silver/gold nanoparticles as seeds and hydrogen peroxide as a reducing agent.