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Wastewater containing synthetic dyes has caused a significant risk to the environment and human health. Among the various methods to treat wastewater, photocatalysis recommends itself as a particularly efficient tool for the removal of dyes from industrial effluents. In this work, Au@Cu2O core@shell nanocrystals with controllable shell thicknesses from 38.1 ± 2.8 (Au@Cu2O-2), 48.1 ± 3.7 (Au@Cu2O-3) to 59.1 ± 4.1 nm (Au@Cu2O-4) have been prepared and immobilized on polyethylene terephthalate (PET) fabrics for applications in photocatalytic degradation of methylene orange (MO). The influence of the shell thickness of Au@Cu2O on the photocatalytic performance of the functionalized PET fabrics has been examined. Among all the samples tested, immobilization of Au@Cu2O-3 rendered PET fabrics the largest photocatalytic activity for MO degradation, achieving an apparent rate constant of MO degradation of 7.43 × 10−3 min−1. A plausible mechanism accounting for the degradation process of MO over the functionalized PET has been proposed based on the results of scavenger experiments. This work has provided a delicate yet practical functional textile paradigm by combining the photocatalytic capability of Au@Cu2O and the adaptable feature of PET fabrics. The findings from this study can deliver a viable idea for the design of versatile textiles with competent photocatalytic capacity for environmental purifications and energy conversion.