In2S3 nanoparticle (NP) decorated self-organized TiO2 nanotube array (In2S3/TiO2 NT) hybrids were fabricated via simple successive ionic layer adsorption and reaction (SILAR) technique. The In2S3 NPs in a size of about 15 nm were found to deposit on the top surface of the highly oriented TiO2 NT while without clogging the tube entrances. The loading amount of In2S3 NPs on the TiO2 NT was controlled by the cycle number of SILAR deposition. Compared with the bare TiO2 NT, the In2S3/TiO2 NT hybrids showed stronger absorption in the visible light region and significantly enhanced photocurrent density. The photocatalytic activity of the In2S3/TiO2 NT photocatalyst far exceeds that of bare TiO2 NT in the degradation of typical herbicide 2,4-dichlorophenoxyacetic acid (2,4-D) under simulated solar light. After 160-min irradiation, almost 100% 2,4-D removal is obtained on the 7-In2S3/TiO2 NT prepared through seven SILAR deposition cycles, much higher than 26% on the bare TiO2 NT. After 10 successive cycles of photocatalytic process with total 1,600 min of irradiation, In2S3/TiO2 NT maintained as high 2,4-D removal efficiency as 95.1% with good stability and easy recovery, which justifies the potential of the photocatalytic system in application for the photocatalytic removal of organic pollutants such as herbicides or pesticides from water.