Developing a photoactive material by combining the characteristics of a wide light response range and effective separation of photogenerated electron-hole pairs remains a huge challenge for the construction of a photoelectrochemical (PEC) sensing platform. Herein, a gold nanoparticle (AuNP)/MoS2/TiO2 composite was prepared through the facile hydrothermal method coupled with an in situ photoreduction technology. Benefiting from both the compositional and structure merits, the composite not only extends the absorption range to visible light but also enhances the photoelectric conversion efficiency by transferring photogenerated electrons into the conduction band of semiconductors from the plasmonic AuNP. Meanwhile, the thiolated aptamers were attached to the surface of AuNP/MoS2/TiO2 composites through the Au-S bonding to construct a visible light driven PEC aptasensor for ultrasensitive detection chloramphenicol (CAP). In the presence of CAP, the aptamers anchored on the surface of the photoactive materials could specifically recognize CAP and interact with it to form a bioaffinity complex with a steric hindrance effect, resulting in the rapid decrease of photocurrent responses. Based on this photocurrent suppression strategy, the constructed PEC aptasensing platform exhibited a high sensitivity with a wide linear range from 5 pM to 100 nM and a low detection limit of 0.5 pM.