The study herein is directed toward the tuning of various properties of recyclable and biocompatible polymer: chitosan (CS) via incorporating the variable wt% of r‐GO in the polymer. The CS/r‐GO polymer nanocomposites (PNCs) are prepared in the form of free‐standing film by solution mixing and casting technique. To search the potential applications, the prepared PNCs are characterized in terms of structural, photoluminescence (PL), surface morphology, optical, and Raman spectra. The crystalline size and microstrain both are enhanced with rise in wt% of r‐GO nanofiller. Raman spectra confirm that as the wt% of r‐GO increases, there is a minor shift toward a smaller wavenumber in the locations of the D, G, and 2D bands, while the intensity ratios ) increase. Field‐emission scanning electron microscopy results are capable of offering details regarding the surface quality for the interface purposes. The characteristic peaks and their broadening in PL spectra, chromaticity coordinates, dominant wavelength, and correlated color temperature are altered with variation of r‐GO wt.%. The optical bandgap, refractive index, and Urbach energy are found to tune with varying the nanofiller wt.%. These results suggest that CS/r‐GO PNC may be the potential candidate for possible application in fabricating the tunable optoelectronic devices.