Antireflective (AR) nanostructures offer an effective, broadband alternative to conventional AR coatings that could be used even under extreme conditions. In this publication, a possible fabrication process based on colloidal polystyrene (PS) nanosphere lithography for the fabrication of such AR structures on arbitrarily shaped fused silica substrates is presented and evaluated. Special emphasis is placed on the involved manufacturing steps in order to be able to produce tailored and effective structures. An improved Langmuir-Blodgett self-assembly lithography technique enabled the deposition of 200 nm PS spheres on curved surfaces, independent of shape or material-specific characteristics such as hydrophobicity. The AR structures were fabricated on planar fused silica wafers and aspherical planoconvex lenses. Broadband AR structures with losses (reflection + transmissive scattering) of <1% per surface in the spectral range of 750–2000 nm were produced. At the best performance level, losses were less than 0.5%, which corresponds to an improvement factor of 6.7 compared to unstructured reference substrates.