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Biology achieves an incredible diversity in structure and function using a comparatively small set of materials and mechanisms. In particular, biology routinely: (i) organizes materials over a hierarchy of length scales using molecular recognition-based self-assembly; and (ii) uses responsive (i.e., switchable) moieties to induce structural transitions in response to external pH and redox cues. Importantly, many cues that induce self-assembly or switching can be imposed electrochemically. In this talk, I will discuss in particular pH-Cue applied to chitosan and collagen-based materials and Redox-Cue applied to quinone-based hydrogels.