The mechanical flexibility of substrates and controllable nanostructures are two major considerations in designing high‐performance, flexible thin‐film solar cells. In this work, we proposed an approach to realize highly ordered metal oxide nanopatterns on polyimide (PI) substrate based on the sol‐gel chemistry and soft thermal nanoimprinting lithography. Thin‐film amorphous silicon (a‐Si:H) solar cells were subsequently constructed on the patterned PI flexible substrates. The periodic nanopatterns delivered broadband‐enhanced light absorption and quantum efficiency, as well as the eventual power conversion efficiency (PCE). The nanotextures also benefit for the device yield and mechanical flexibility, which experienced little efficiency drop even after 100,000 bending cycles. In addition, flexible, transparent nanocone films, obtained by a template process, were attached onto the patterned PI solar cells, serving as top anti‐reflection layers. The PCE performance with these dual‐interfacial patterns rose up to 8.17%, that is, it improved by 48.5% over the planar device. Although the work was conducted on a‐Si:H material, our proposed scheme can be extended to a variety of active materials for different optoelectronic applications.