Photocatalysis is an efficient approach to degrade hydrogen sulfide (H S) and titanium dioxide (TiO ) is commonly used as a catalyst for H S degradation. However, the low separation rate of photoinduced carriers and low gas adsorption ability of TiO limit its H S photocatalytic decomposition rate. In this paper, single-crystalline TiO nanowires are assembled on one-dimensional carbon nanofibers (CNFs) and a tunable metal-organic framework (MOF) coating is fabricated on the surface of the TiO nanowires using a versatile step-by-step self-assembly strategy. The excellent photocatalytic properties of the resulting membrane originate from the ability of the CNFs to rapidly transport charge carriers and the high and regenerable H S adsorption ability of the MOF. The photocatalytic mechanism of the as-prepared material was also discussed. Therefore, this work provides a promising method to improve the photocatalytic performance of H S degradation.