Osmanthus fragrance-loaded chitosan nanoparticles (OF-NPs) were prepared via complex coacervation successfully. Then, the OF-NPs were applied in the cotton fabrics directly. The microstructures of OF-NPs were characterized by dynamic light scattering (DLS), transmission electron microscopy (TEM), Fourier transformation infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA). The sustained property of the cotton fabrics treated with OF-NPs was investigated with scanning electron microscopy (SEM) and gas chromatographymass spectrometry (GC-MS). The common OF was also treated on fabrics for the parallel comparison. TEM and DLS displayed that the spherical OF-NPs kept about 130 nm and dispersed evenly. FTIR confirmed that OF had been interacted with chitosan via the hydrogen bonds. TGA demonstrated that the thermal stability of OF-NPs had been improved in contrast to OF and the loading content of OF was as high as 12.05%. SEM and GC-MS displayed that the cotton fabrics treated by OF-NPs had an excellent washing resistance. Overall, nanoencapsulation with CS-TPP will provide an excellent method for releasing fragrance.