Assembling optical active nanostructures into polymer matrices holds promise for the design of functional materials with controlled light-matter interactions, which finds applications such as sensors and flexible photovoltaics. We present various methodologies for the control of the plasmonic properties of gold nanorods and the photoluminescence of quantum dot (QD). First, electrochromic hybrid systems with electrochemical modulation of plasmon resonance were designed by direct polymerizing electroactive polymers around gold nanorods. The plasmon tuning behavior, resulted from polymer’s refractive index change, varied when different electroactive polymers were used. For example, a dual-responsive system with the plasmon mode reversibly modulated through electric potential and pH was realized when polyaniline served as the outer shell and a maximum shift of the longitudinal plasmon mode of 149 nm was obtained. Another electrochemical modulated plasmon tuning system with narrow visible-near infrared absorption bands was also demonstrated using a transmissive polymer poly[(3,4-propylenedioxy)pyrrole]. Overall, these core-shell nanostructures with electrochemical plasmonic tunability allow for the fine control of the optical and electrochemical properties of plasmon response. Second, we developed a new method for enhancing photoluminescence from QDs/polymer nanocomposite through the control of the degree of film dewetting. The dewetted films were found to have increased amounts of scattering, which resulted in up to a 5-fold enhancement of the film emission. A unique photopatterning strategy was also presented based on the aforementioned method.