Broadband antireflection (AR) coatings are essential elements for improving the photocurrent generation of photovoltaic modules or the enhancement of visibility in optical devices. In this paper, we report a hybrid nanostructured antireflection coating combination that is a clean and efficient method for fabricating a nanostructured antireflection coating (ARC). A multilayer thin-film was introduced between the ARC and substrate to solve the significant problem of preparing nanostructured ARCs on different substrates. In this way, we rebuilt a gradient refractive index structure and optimize the antireflective property by simply adjusting the moth-eye structure and multilayers. Subwavelength-structured cone arrays were directly patterned using a self-assembled single-layer polystyrene (PS) nanosphere array as an etching mask. Nanostructure coatings exhibited excellent broadband and wide-angle antireflective properties. The bottom-up preparation process and hybrid structural combination have the potential to significantly enhance the broadband and wide-angle antireflective properties for a number of optical systems that require high transparency, which is promising for reducing the manufacturing cost of nanostructured AR coatings.