Part of the light incident on all transparent materials is reflected. This reflection arises from the abrupt change in the refractive index at the interface of two media. The cornea of some nocturnal moths has a structure with a repeating pattern of less than 250 nm and a physical depth of less than 200 nm. These submicrostructured surfaces can greatly reduce reflection, helping conceal the inset from hungry predators. We report a simple bio-inspired self-assembly technique for fabricating artificial moth-eye antireflective coatings. Non-close-packed colloidal crystals with remarkable large hexagonal domains are created by a spin-coating technology, which is based on shear-aligning colloidal silica particles suspended in non-volatile triacrylate monomers. The resulting polymer-embedded colloidal crystals exhibit highly ordered surface modulation and can be used directly as templates to cast poly(dimethylsiloxane) (PDMS) molds. Polymer (e.g., PMMA and polystyrene) and glass antireflective coatings can then be molded against PDMS using traditional polymerization and sol-gel technologies. The depth of the micropatterns can be adjusted by plasma-etching of the original colloidal crystal-polymer nanocomposite. Using the above colloidal self-assembly and micromolding techniques, large-area (up to 8-inch diameter, limited only by the substrate size) moth-eye antireflective coatings have been created on both planar and curved substrates. The microstructured coatings exhibit much lower reflectivity than bare films and the optical reflection matches with the theoretical prediction using effective medium theory.