We aim at exploring how nature performs complicated redox reactions constituting key processes in the environment and life, like biomass degradation and or cellular respiration. At the heart of such processes are often redox biocatalytic metalloproteins which present the main inspiration for our mechanistic investigations. In our research mission, we want to understand how we can harness and further engineer the unrivaled efficiency of such natural biological systems towards the development of artificial biohybrid systems applicable in bioelectronic devices. Methodologically, we employ the combination of experimental techniques including advanced Raman spectroscopy, electrochemistry, and protein engineering. Specifically, surface-enhanced resonance Raman spectro-electrochemistry allows us to correlate the structural information of the molecule interfaced on electrodes with its redox functionality.