We demonstrate control, via electro-hydrodynamic (EHD) induced polymer instabilities and nanoparticle mobility, of hierarchical fractal arrangements of gold nanoparticles on patterned thin polymer films. The induced changes in the film curvature enhance fractal formation for high and not for low mobility nanoparticles. The high mobility nanoparticles cluster in circular fractal networks on the rims of a hexagonally ordered array of EHD-induced polymer peaks. These arrangements exhibit plasmonic properties for surface-enhanced Raman scattering (SERS) spectroscopy.