Fresnel reflection at the boundary between two media of differing refractive indices is a major contributing factor to the overall loss in mid-infrared optical systems based on high-index materials such as chalcogenide glasses. In this paper, we present a study of broadband antireflective moth-eye structures directly nanoimprinted on the surfaces of arsenic triselenide (As2Se3)-based optical windows. Using rigorous coupled-wave analysis, we identify a relief design optimized for high transmittance (<1% reflectance) at 6 μm, which when nanoimprinted features a transmittance improvement (ΔT > 12%) in the 5.9–7.3 μm spectral range as well as improved omnidirectional properties. Finally, we demonstrate the adaptability of nanoimprinted surface reliefs by tailoring the nanostructure pitch and height, achieving both extremely broadband antireflective and highly efficient antireflective surface reliefs. The results and methods presented herein provide an efficient and scalable solution for improving the transmission of bulk optics, waveguides, and photonic devices in the mid-infrared.