We report on the fabrication of nanostructures built of actin using the Atomic Force Microscopy and molecularly organised substrata, i.e. HOPG and mica. We obtained both ‘paracrystalline rafts’ of actin adsorbed onto hydrophobic HOPG, as well as selective adsorption with nano-scale definition obtained on mica by taking advantage of the propensity of actin to seek sites of lowest energy configuration at interfaces. In the latter mode, we obtained circular patterns of 100-500 nm diameter. Filamentary structures on a hydrophobic substrate form paracrystalline rafts that can readily be manipulated on the nano-scale, while adsorption on a hydrophilic surface suggests that tailored interfaces will impose structural predictability.