Use of colloidal suspensions to generate structural colors has the potential to reduce the use of toxic metals or organic pigments in inkjet printing, coatings, cosmetics, and other applications, and is a promising avenue to create large-scale nanostructures that produce long-lasting colors. However, expanded use of structural colors requires a reduction in coffee-ring effects during printing, which currently requires intricately patterned substrates or high particle concentrations, and diversification of colors to compete with conventional printing inks. Here, we treat substrate surfaces with cold plasma to facilitate spontaneous assembly of particles into colloidal nanostructures, reducing the need for highly concentrated particle suspensions. Moreover, by employing binary mixtures, we can tune the lightness of the hue produced or change the hue itself, allowing us to cover wider regions of color space. We demonstrate the use of this cold-plasma approach on a variety of substrates, favoring substrate diversity on which printing can be performed. This methodology enables creation of high-resolution, complex designs and opens a path for extending the limits of anticounterfeiting applications by using binary mixtures.

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.