Structural systems deteriorate due to excessive deformation and corrosive environments. If damage is left undetected, they can propagate to cause sudden collapse. However, one of the main difficulties of monitoring damage progression is that, for example, excessive/plastic deformation and corrosion are drastically different physical processes. Strain is a mechanical phenomenon, whereas corrosion is a complex electrochemical process. The current strategy for structural health monitoring (SHM) is to use either different types of sensors or to employ system identification for quantifying overall changes to the structure. In this study, an alternative SHM paradigm is proposed in that a single, multifunctional material would be able to selectively sense different but simultaneously occurring structural damage. In particular, a photoactive and self-sensing thin film was developed for monitoring strain and corrosion. Another unique aspect was that the films were self-sensing and did not depend on external electrical energy for operations. First, the thin films were fabricated using photoactive poly(3-hexylthiophene) (P3HT) and other functional polymers using spin-coating and layerby- layer assembly. Second, the fabricated thin films were interrogated using an ultraviolet-visible (UV-Vis) spectrophotometer for quantifying their optical response to applied external stimuli, such as strain and exposure to pH buffer solutions. Lastly, the multifunctional thin films were tested and validated for strain and pH sensing. Interrogation of these separate responses was achieved by illuminating the thin films different wavelengths of light and then measuring the corresponding electrical current generated.