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Coupling appropriate semiconductor nanoparticles with massive surface-area support has become a promising but challenging strategy to photocatalyst design for enhanced photocatalytic activity in environmental cleaning applications, owing to the severe aggregation issues of nanoparticles. Herein, the atomic layer deposition (ALD) approach was applied to uniformly disperse ultrafine Cu 2 O nanoparticles (5–10 nm) on metal-organic frameworks without aggregation, forming NH 2 -MIL-101(Fe)/Cu 2 O nanocomposite photocatalysts. The Cu 2 O mass within the nanocomposites can be well controlled by merely adjusting the ALD cycles. The optimal NH 2 -MIL-101(Fe)/Cu 2 O displays a high photodegradation efficiency of 92% for RhB and excellent stability under visible light. The reaction kinetics and photocurrent response experimental results reveal that the optimal NH 2 -MIL-101(Fe)/Cu 2 O photocatalyst exhibits effective charge separation/transfer and suppressed recombination rate of charge carriers, which will significantly increase the solar light utilization efficiency and photocatalytic activity. We believe the presented photocatalyst synthesis strategy here can be generalized to construct other photocatalysts for various photocatalytic applications. [ABSTRACT FROM AUTHOR]