Nanostructured materials producing structural colors have great potential in replacing toxic metals or organic pigments. Electrophoretic deposition (EPD) is a promising method for producing these materials on a large scale, but it requires improvements in brightness, saturation, and mechanical stability. Herein, we use EPD assembly to codeposit silica (SiO 2 ) particles with precursors of synthetic melanin, polydopamine (PDA), to produce mechanically robust, wide-angle structurally colored coatings. We use spectrophotometry to show that PDA precursors enhance the saturation of structural colors and nanoscratch testing to demonstrate that they stabilize particles within the EPD coatings. Stabilization by PDA precursors allows us to coat flexible substrates that can sustain bending stresses, opening an avenue for electroprinting on flexible materials.