Biomanufacturing of ethylene is particularly important for modern society. Cyanobacterial cells are able to photosynthesize various valuable chemicals. A promising platform for next‐generation biomanufacturing, the semiconductor‐cyanobacterial hybrid systems are capable of enhancing the solar‐to‐chemical conversion efficiency. Herein, the native ethylene‐producing capability of a filamentous cyanobacterium Nostoc sphaeroides is confirmed experimentally. The self‐assembly characteristic of N. sphaeroides is exploited to facilitate its interaction with InP nanomaterial, and the resulting biohybrid system gave rise to further elevated photosynthetic ethylene production. Based on chlorophyll fluorescence measurement and metabolic analysis, the InP nanomaterial‐augmented photosystem I activity and enhanced ethylene production metabolism of biohybrid cells are confirmed, the mechanism underlying the material‐cell energy transduction as well as nanomaterial‐modulated photosynthetic light and dark reactions are established. This work not only demonstrates the potential application of semiconductor‐N. sphaeroides biohybrid system as a good platform for sustainable ethylene production but also provides an important reference for future studies to construct and optimize nano‐cell biohybrid systems for efficient solar‐driven valuable chemical production.