LAUSR

The construction and optimization of an effective photocatalyst for photodegradation of persistent recalcitrant organic remains challenging. In this work, MIL‐101(Cr)‐based nanocomposites (AgI@MCr) are proposed to be fabricated by a simple, green solvent, and room temperature in situ preparation strategy, achieving a highly efficient photocatalytic degradation of organic dye rhodamine B (RhB) molecule under visible light irradiation. Extensive characterization (XRD, FTIR, N2 adsorption–desorption, SEM and EDS, TG, XPS, UV–vis DRS, PL, transient photocurrent, and EIS) confirmed the composite material's structure, morphology, elemental composition, and optical characteristics. Among all the prepared nanocomposites, AgI@MCr‐2 demonstrates outstanding photocatalytic performance for RhB with a removal efficiency of 95.4% within 70 min, and a reaction kinetics of 0.0392 min−1, superior to pristine AgI or MIL‐101(Cr), and also shows excellent durability, retaining over 80% RhB degradation efficiency after four cycles. Remarkably, the significant enhancement is attributed to the built interfacial contact and synergistic effect between substances in the nanocomposite, high specific surface area, strong visible light–harvesting capacity, low bandgaps, and high electron–hole pair separation. In addition, a possible degradation route for the AgI@MCr nanocomposite is further proposed using various analysis techniques. This study provides valuable references for developing effective multicomponent MOF‐based photocatalytic composite materials for dyeing wastewater treatment and environmental remediation.