Conjugated polymers (CPs) have become essential to a diverse array of fields, ranging from biosensing to photovoltaics to optoelectronic materials. Given their widespread use, there is a growing need for variants whose functions may be modulated via exogenous stimuli. Alteration of CP structure could effect the desired changes and may be actuated in response to (1) chemical, (2) electrochemical, (3) photochemical, or (4) thermal impetuses. In this Perspective, we present a review of CPs reported to respond to chemical, electrochemical, and photochemical stimuli along with our own efforts using thermal stimuli. A particular emphasis has been directed toward structurally dynamic CPs that exhibit changes in their electronic properties, which could enable access to new classes of smart and other functional materials. During the course of our discussion, we consider the advantages and disadvantages inherent to each of the aforementioned methods, along with the potential applications of the polymers derived therefrom. We conclude this Perspective with a brief overview of the accomplishments in this nascent field, reflecting upon the unconquered challenges and contemplating the opportunities present for future discoveries involving structurally dynamic CPs.