A novel CC@MoS2-Ag3PO4 heterostructure, composed of Ag3PO4 nanoparticles decorated MoS2 nanosheets on carbon fiber cloth (CC), is fabricated by a simple hydrothermal method and a successive ionic layer absorption reaction. The CC@MoS2-Ag3PO4 heterostructure displays an excellent photocatalytic activity of 96% degradation rate for RhB solution under simulated daylight, which is more than 10 times as much as that of pure Ag3PO4 or MoS2. The CC@MoS2-Ag3PO4 heterostructure with optimized photoactivity is investigated by optical and electrochemical measurements. The CC@MoS2-Ag3PO4 heterostructure can not only broaden the photo response range of MoS2, but also alleviate the photodegradation of Ag3PO4, and the easily separated CC provides a proper conductive substrate and rapid charge transfer channels. The probable photocatalytic mechanism of CC@MoS2-Ag3PO4 heterostructure is discussed in detail. Therefore, the CC@MoS2-Ag3PO4 heterostructure with high efficient photocatalytic performance and easy separation is a promising photocatalytic material.