We employ principles derived from biomineralization to assemble functional nanoscale inorganic materials onto flexible polymer substrates under low-temperature, benign chemical conditions. Our biomimetic approach involves the selective functionalization of polymer surfaces to create regions of differing surface energy which can promote heterogeneous nucleation in designated regions while suppressing it in others. Specifically, ZnO is grown into ordered microarrays on flexible polycarbonate films and polyester filaments directly out of aqueous solutions. The resulting block, checkerboard, and grid shaped microarrays consist of either ZnO nanorods or microplates with feature sizes down to 4 mu m. The approach reported is general does not require traditional lithography, uses no seed layers or self-assembled monolayers, and can be easily applied to a variety of planar or three-dimensional polymer substrates enabling numerous applications in flexible macroelectronics and smart textiles.