Optoelectronic nanoscale devices have wide applications in chemical, biological, and medical technologies. Improving the performance efficiency of these devices remains a challenge. Performance is mainly dictated by the structure and characteristics of the semiconductor materials. Once a nanodevice is fabricated, its efficiency is determined. The key to improving efficiency is to control the interfaces in the device. In this article, we describe how the piezo-phototronic effect can be effectively utilized to modulate the band at the interface of a metal/semiconductor contact or a p–n junction to enhance the external efficiency of many optoelectronic nanoscale devices such as photodetectors, solar cells, and light-emitting diodes (LEDs). The piezo-phototronic effect can be highly effective at enhancing the efficiency of energy conversion in today’s green and renewable energy technology without using the sophisticated nanofabrication procedures that have high cost and complexity.