In this study, we successfully synthesized a novel composite material UiO-66/polyacrylate (UiO/PA) by suspension polymerization and in situ growth of metal−organic frameworks (MOFs). Due to the control of heterogeneous nucleation and firm growth, nano-UiO-66 with a diameter of only 400 nm has been reduced by about 90%, resulting in lower transfer resistance, effective separation of photogenerated carriers, and more catalytic active sites exposed. Under visible light irradiation, UiO/PA with 48.7% loading can almost completely degrade rhodamine B (RhB) in 120 min and the corresponding degradation rate constant of RhB reached 0.0203 min −1 from 0 min −1 . After easy filtration and five cycles, the degradation rate is still above 85%. This study can provide new insights into effectively improving the photocatalytic performance of MOFs.