Imatinib (IMB), a widely employed anticancer agent, poses significant environmental concerns due to its release into aquatic ecosystems via pharmaceutical industries and hospital effluents, contributing to water source contamination and consequential impacts on both human and animal health. In light of this, a novel bimetallic MIL-53(Co-Fe)@MIL-53(Ni)/TiO2 composite material has been synthesized utilizing hydrothermal approaches for the efficient adsorption and photodegradation of IMB. Comparative assessments were conducted between this composite and MIL-53(Ni), bimetallic MIL-53(Co-Fe)@MIL-53(Ni), bare TiO2 for their respective capacities in IMB removal through adsorption and photodegradation. Remarkably enhanced efficacy was observed in the synthetic composite's performance for both adsorption and photodegradation, surpassing that of other compounds. Through systematic exploration, critical parameters influencing the adsorption and photodegradation processes were meticulously examined and subsequently optimized utilizing experimental design strategies. Optimal conditions led to the identification of a pseudo-second-order kinetic model for IMB adsorption with a notable rate constant of 8.39 and an equilibrium time of 75 min. The adsorption process conformed favorably to the Freundlich isotherm, as evidenced by the Freundlich constant of 25.498 mg g−1 and adsorption intensity of 2.09. These values underscored the heightened affinity of the synthetic composite relative to IMB, ascribed to the favorable absorption. A complementary investigation into the kinetics of IMB photodegradation unveiled a substantially elevated rate constant of 0.0407 min−1, coupled with a proper half-life of 17.03 min. These collective findings validate the exceptional capacity of the synthesized composite for dual-mode IMB elimination, encompassing both adsorption and photodegradation pathways. This advancement holds significant promise for addressing the environmental repercussions of IMB contamination and points to the potential for broader applications in wastewater treatment and ecological restoration endeavors.