Collagen is a building block that can be hierarchically assembled into diverse morphological structures that are dynamically adaptive in response to external cues. Materials scientists have limited capabilities of guiding the emergence of collagen’s hierarchical organization to recapture the richness of its biological structure and function in the lab. In a new report now published in Science Advances, Miao Lei, and a research team in materials science, medicine, and science and technology, in China and the U.S., described an electro-assembly pathway to build an intermediate molten fibril state for collagen. The intermediate state was structurally made of partially aligned and reversibly associated fibrils with limited hierarchical structure. They reversibly reconfigured the molten fibrils to offer dynamic properties such as stimuli-based stiffening, contracting, self-healing and self-shaping character and guided the molten fibrils to further assemble and recapitulate structural features of native collagen. The outcomes provide hitherto unidentified methods to tailor collagen-based biomedical materials.