Electrochemical activation of glassy carbon, carbon paper and functionalized carbon nanotubes via high-applied-potential cyclic voltammetry leads to the formation of adsorbed, redox active functional groups and increased active surface area. Electrochemically activated carbon electrodes display enhanced activity toward nicotinamide adenine dinucleotide (NADH) oxidation, and more importantly, dramatically improved adsorption of bioelectrochemically active azine dyes. Adsorption of methylene green on an electroactivated carbon electrode yields a catalyst layer that is 1.8-fold more active toward NADH oxidation than an electrode prepared using electropolymerized methylene green. Stability studies using cyclic voltammetry indicate 70% activity retention after 4000 cycles. This work further facilitates the electrocatalysis of NADH oxidation for bioconversion, biosensor and bioenergy processes.