In this work, ZnO quantum dots (ZnOQD) were synthesized by Sol–gel synthesis and impregnated on polylactic acid (PLA) knitted fabric through self-assembly of different cycles from layer-by-layer (LBL) using cationic agent Poly(diallydimethylammonium chloride) (PDDA). Then, morphological, chemical and photocatalytic properties were studied. The results demonstrate that the synthesis provided 8 nm Wurtzite-type ZnO nanoparticles. In addition, X-ray photoelectron spectroscopy (XPS) spectra, X-ray diffraction (XRD) and scanning electron microscopy (SEM) proved the inclusion of ZnOQD on the surface of PLA matrix, which allowed the evaluation of its photocatalytic properties, therefore, coated PLA with five cycles of ZnOQD obtained the best result for degrading 85% of the dye Rhodamine B (RhB) in 360 min under UV radiation, in addition to its reusability for another five cycles of photocatalytic activity.