We report herein a versatile new approach for improving the photodegradation performance of UiO-66 by introducing 2-methylimidazole through a straightforward in situ one-pot solvothermal method. The resultant complex UiO-66-M-0.7 has demonstrated a reaction rate constant of 0.0183 min(-1)in the photodegradation of rhodamine B under visible light, which is 69.4% higher than that with unmodulated UiO-66. Further investigation has confirmed that the improved activity can be attributed to enhanced adsorption of the dye by the photocatalyst during the adsorption-desorption equilibrium. The main active species involved in the photodegradation process have been identified as h(+) and O-2(-)center dot. In addition, the complex has shown ideal stability in recycling tests and excellent activity in the degradation of methylene blue. This study provides a novel perspective for the future design of various photocatalysts with superior performance. GRAPHIC ABSTRACT 2-Methylimidazole-modulated UiO-66 exhibits increased catalytic performance in the photodegradation of rhodamine B (RhB) under visible light because of enhanced adsorption of RhB on the catalyst during the adsorption-desorption equilibrium. [GRAPHICS]