The necessity for reliable and efficient multifunctional optical and optoelectronic devices is always calling for the exploration of new fertile materials for this purpose. This study leverages the exploitation of dyed environmentally friendly biopolymeric thin films as a potential optical absorber in the development of multifunctional opto-(electronic) and solar cell applications. Uniform, stable thin films of dyed chitosan were prepared using a spin-coating approach. The molecular interactivity between the chitosan matrix and all the additive organic dyes was evaluated using FTIR measurements. The color variations were assessed using chromaticity (CIE) measurements. The optical properties of films were inspected using the measured UV-vis-NIR transmission and reflection spectra. The values of the energy gap and Urbach energy as well as the electronic parameters and nonlinear optical parameters of films were estimated. The prepared films were exploited for laser shielding as an attenuated laser cut-off material. In addition, the performance of the prepared thin films as an absorbing organic layer with silicon in an organic/inorganic heterojunction architecture for photosensing and solar energy conversion applicability was studied. The current-voltage relation under dark and illumination declared the suitability of this architecture in terms of responsivity and specific detectivity values for efficient light sensing applications. The suitability of such films for solar cell fabrications is due to some dyed films achieving open-circuit voltage and short-circuit current values, where Saf-dyed films achieved the highestVoc(302 mV) while MV-dyed films achieved the highestJsc(0.005 mA/cm2). Finally, based on all the obtained characterization results, the engineered natural cost-effective dyed films are considered potential active materials for a wide range of optical and optoelectronic applications.