Metalloenzymes are nature's own catalysts and offer as such endless inspirational source for the chemists seeking selectivity in transformations. Metalloenzymes involved in oxidoreduction processes have specific subunits dedicated to electron and proton transfer, and these so‐called redox cofactors perform highly orchestrated redox events. This minireview offers a perspective on the development of biomimetic and bioinspired innovative approaches interfacing redox cofactors engineering with metal‐based catalysis, nanochemistry, light‐activation, supramolecular chemistry and artificial metalloenzymes to devise and build new synthetic systems using nature's finest electron transfer tools. Cofactors are key factors: This Minireview offers a perspective on the development of biomimetic and bioinspired strategies interfacing redox cofactors engineering with topics such as metal‐based catalysis, nanochemistry, light‐activation, supramolecular chemistry and artificial metalloenzymes to devise and build new synthetic systems using nature's finest electron transfer tools.