The intricate, siliceous exoskeleton of many marine diatoms (single-celled phytoplankton) is decorated with an array of sub-micron, quasi-ordered pores that are known to provide protective and multiple life-sustaining functions. However, the optical functionality of any given diatom valve is limited because valve geometry, composition, and ordering are genetically programmed. Nonetheless, the near- and sub-wavelength features of diatom valves provide inspiration for novel photonic surfaces and devices. Herein, we explore the optical design space for optical transmission, reflection, and scattering in diatom-like structures by computationally deconstructing the diatom frustule, assigning and nondimensionalizing Fano-resonant behavior with configurations of increasing refractive index contrast (Δn), and gauging the effects of structural disorder on the resulting optical response. Translational pore disorder, especially in higher-index materials, was found to evolve Fano resonances from near-unity reflection and transmission to modally confined, angle-independent scattering, which is key to non-iridescent coloration in the visible wavelength range. High-index, frustule-like TiO2 nanomembranes were then designed to maximize backscattering intensity and fabricated using colloidal lithography. These synthetic diatom surfaces showed saturated, non-iridescent coloration across the visible spectrum. Overall, this diatom-inspired platform could be useful in designing tailored, functional, and nanostructured surfaces for applications in optics, heterogeneous catalysis, sensing, and optoelectronics.