A method of fabricating horizontally aligned ZnO nanowire (NW) arrays with full control over the width and length is demonstrated. A cross-sectional view of the NWs by transmission electron microscopy shows a “mushroom-like” structure. Novel monolithic multisegment superstructures are fabricated by making use of the lateral overgrowth. Ultralong horizontal ZnO NWs of an aspect ratio on the order of ten thousand are also demonstrated. These horizontal NWs are lifted off and transferred onto a flexible polymer substrate, which may have many great applications in horizontal ZnO NW-based nanosensor arrays, light-emitting diodes, optical gratings, integrated circuit interconnects, and high-output-power alternating-current nanogenerators.