The objective of this study was to identify chitosan formulations suitable for sustainable functional integration into composite materials. To this end, the influence of solvent type (acetic acid and lactic acid) and chitosan molecular weight on film formation, rheological behavior, thermal response, thermo-optical properties, chemical structure, and piezoelectric performance was systematically investigated. Optimized casting and drying procedures produced transparent, homogeneous, and mechanically stable films suitable for comprehensive characterization. Rheological and thermo-optical analyses demonstrated that solvent selection strongly influenced polymer network formation and molecular mobility. Films prepared using acetic acid exhibited denser and stiffer polymer networks with improved dimensional stability, whereas lactic acid produced more flexible and elastic films. Thermogravimetric analysis revealed only minor differences in the intrinsic thermal stability of the investigated films, while FTIR confirmed that the solvent systems did not alter the chemical structure of chitosan. Electrical measurements carried out whilst the system was subjected to periodic mechanical excitation revealed weak but equally periodic electrical signals, which demonstrate a sensor functionality. These results demonstrate that chitosan films possess tunable structural, thermal, and potential mechanoelectrical sensor properties and highlight their potential as sustainable, functionally integrated components in composite material systems.