Immobilization of inorganic metal quantum dots (especially, noble transition metals) onto organic polymers to synthesize nanometal−polymer composites (NMPCs) has attracted considerable attention because of their advanced optical, electrical, catalytic/photocatalytic, and biological properties. Herein, novel, highly efficient, stable, and visible light-active NMPC photocatalysts consisting of silver quantum dots (Ag QDs) immobilized onto polymeric chitosan−polyethylene oxide (CTS−PEO) blend sheets have been successfully prepared by an in situ self-assembly facile casting method as a facile and green approach. The CTS−PEO blend polymer acts as a reducing and a stabilizing agent for Ag QDs which does not generate any environmental chemical pollutant. The prepared x wt % Ag QDs/CTS−PEO composites were fully characterized through X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy (TEM), thermogravimetric analysis, and UV/visible spectroscopy. The characterization results indicated the successful synthesis of the Ag QDs/CTS−PEO composites by the interactions and complexation between x wt % Ag QDs and CTS−PEO blend sheets. TEM images revealed small granules randomly distributed onto the CTS−PEO blend sheets, indicating the immobilization of Ag QDs onto CTS−PEO composites. The presence of a surface plasmon resonance (SPR) band and the shifting of the absorption edge toward higher wavelengths in the UV/vis spectra indicated the formation of x wt % Ag QDs/CTS−PEO composites. The Ag QDs in the polymeric blend matrix led to remarkable enhancement in the optical, thermal, electrical, and photocatalytic properties of x wt % Ag QDs/CTS−PEO composites. The photocatalytic efficiency of the prepared composites was evaluated by the photodegradation of p-nitrophenol (PNP) under simulated sunlight. The maximum photocatalytic degradation reached 91.1% efficiency within 3 h for the 12.0 wt % Ag QDs/CTS−PEO photocatalyst. Generally, the Ag QDs immobilized onto CTS−PEO blend composites significantly enhance the SPR effect and the synergistic effect and reduce the band gap, leading to a high photocatalytic activity.