Eumelanins, the characteristic black, insoluble, and heterogeneous biopolymers of human skin, hair, and eyes, have intrigued and challenged generations of chemists, physicists, and biologists because of their unique structural and optoelectronic properties. Recently, the methods of organic chemistry have been combined with advanced spectroscopic and imaging techniques, theoretical calculations, and methods of condensed-matter physics to gradually force these materials to reveal their secrets. Herein we review the latest advances in the field with a view to showing how the emerging knowledge is not only helping to explain eumelanin functionality, but may also be translated into effective strategies for exploiting their properties to create a new class of biologically inspired high-tech materials.