Nature is replete with extraordinary materials that can grow, move, respond, and adapt. In this talk I will describe our ongoing efforts to develop advanced polymeric materials, inspired by nature. First, I will describe my group’s efforts to develop ultrastiff, ultratough materials inspired by the byssal materials of marine mussels. These adhesive contacts allow mussels to secure themselves to rocks, wood, metals and other surfaces in the harsh conditions of the intertidal zone. By developing a foundational understanding of the structure-mechanics relationships and processing of the natural system, we can design high-performance materials that are extremely strong without compromising extensibility, as well as macroporous materials with tunable toughness and strength. In the second half of the talk, I will describe new efforts to exploit light as a means of remote control and power. By leveraging the phototransduction pathways of highly-absorbing, negatively photochromic molecules, we can drive the motion of amorphous polymeric materials as well as liquid flows. These innovations enable applications in packaging, connective tissue repair, soft robotics, and optofluidics.