A nanopatterning technique using nanostamps that provides a facile process to create a nature-inspired moth-eye structure achieving high transmittance in the visible range as well as a self-cleaning effect is reported. Commercially available perfluoropolyether (PFPE) and NOA63 as the mold resin and second replica mold material, respectively, play an important role in fabricating the structure. The structure is found to increase transmittance up to 82% at 540 nm and contact angle up to 150°, representing superhydrophobicity even without the aid of a fluorinated self-assembled monolayer (SAM) coating. The resulting solid-state dye-sensitized solar cells (ssDSSCs) with moth-eye structures show enhancement of efficiency to 7.3% at 100 mW cm−2, which is among the highest values reported to date for N719 dye-based ssDSSCs. This nature-inspired nanopatterning process could be used for improving light harvesting in any type of photovoltaic cell, and it produces superhydrophobic surfaces, which in turn lead to self-cleaning for long-term stability.