Photocatalysts, such as TiO2, are widely used in photoreduction. However, drawbacks like their wide band gap and short carrier lifetime lead to lower efficiencies with their use. Introducing defects and forming heterostructures of TiO2 could extend the carrier’s light-harvesting range from UV to visible light and enhance its lifetime. Herein, an electron-beam irradiation-defected TiO2 was induced in MIL-88B(Fe). The structure of the material was characterized using XRD, FT-IR, TEM, HRTEM, and XPS techniques. Remarkably, TiO2 under 300 kGy electron-beam irradiation performed the best with a series of 0, 100, 300, and 500 kGy irradiation ratios. PL and UV–vis DRS were utilized to measure the material’s optical properties. The introduction of MIL-88B(Fe) expanded the light response range, reduced the optical band gap, and lengthened the carrier lifetime of the defective TiO2 composite photocatalysts, resulting in superior TC photoreduction capabilities of 88B5%300, which degraded 97% of tetracycline (10 mg/L) in water after 120 min.