Dyeing wastewater has caused serious environmental problems nowadays. In this work, nickel–phosphorus plating–titanium dioxide (Ni-P-TiO2) electroless plating polyimide (PI) fabric was fabricated as an excellent visible light response composite. First, polyaniline (PANI) was in situ polymerized on the surface of the PI fabric. Second, PANI reduced palladium ions to be active seeds for initiating electroless plating of Ni-P-TiO2 layer. Finally, the Ni-P-TiO2/PANI/PI fabric with all-in-one structure was prepared, which can effectively overcome the drawbacks of poor loading fastness and insensitivity to visible light response. It was characterized by scanning electron microscopy, energy-dispersive spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, thermogravimetric analysis, and ultraviolet–visible diffuse reflectance spectroscopy. The photocatalytic activity was evaluated by degrading reactive blue 19, methylene blue, and reactive red (M-3BE) under visible light irradiation. The results show that the degradation rates of the all three dyes were over 91% with robust cycle stability for repeated 5 cycles of use. The possible photocatalytic degradation mechanism of fabrics was also proposed based on free radical and hole removal experiments.