Taking inspiration from a variety of creatures found in nature, this thesis demonstrates a new class of materials designed for light capture and guidance. Through the facile method of waveguide self-inscription developed herein, the arrangement of these self-generated light channels can be influenced to produce complex architectures. Inspired by the arrangement of ommatidia found in arthropodal eyes, this was first demonstrated through the fabrication of a radial arrangement of waveguides. This resulted in a thin, polymer film which demonstrated a continuous, panoramic field of view (FOV) able to successfully control the light of a light emitting diode (LED). Moving to more complex architecture, waveguides self-generated in a conical geometry were fabricated. More closely reminiscent of the geometry seen in arthropodal eyes, this waveguide architecture demonstrated a seamless omnidirectional FOV and enhanced imaging capabilities in conjunction with a CMOS camera chip. Lastly, using the method of waveguide self-inscription with an electroactive hydrogel precursor, remote controllable light guiding architectures, as inspired by deep sea creatures, are designed and fabricated. The application of an electric field, in conjunction with the stimuli-responsive waveguides, allows for precise control of the waveguide structures and therefore control over the waveguided light. / Thesis / Doctor of Philosophy (PhD)