Removal of organic pollutants from wastewater remains a significant challenge. Hence, we report a series of novel MOFs based BixTiy‐BTC photocatalysts synthesized by hydrothermal method for decontamination of 1,1‐Dimethylhydrazine (UDMH). The preparation parameters of MOFs were optimized, the best catalytic performance was achieved by adjusting the Bi/Ti molar ratio to 1 : 3, with Bi1Ti3‐BTC a photocurrent density of 0.35 mA/cm2 was reached. The morphology and composition of the materials were analyzed, titanium doping increased the specific surface area. Bi1Ti3‐BTC was loaded with magnetic nano‐Fe3O4, which prevented agglomeration of Bi1Ti3‐BTC and increased the specific surface area, thus improving photocatalytic activity. The band gap structure of the semiconductor materials was estimated by UV‐Vis and XPS valence band spectra, while the separation efficiency of photogenerated carriers was investigated by photocurrent density and PL (Photoluminescence) spectrum. The photocatalytic degradation rate of UDMH rapidly decreased after addition of EDTA, indicating that h+ was the main active species in the photocatalytic degradation process. The photocatalytic removal efficiency of UDMH with Bi1Ti3‐BTC/Fe3O4 at a concentration of 0.5 g/L reached 97.58 % after illumination for 180 min, and after 210 min near quantitative degradation was observed.