In this presentation, my objective is to share my research exposure on carbon nanomaterial-pyrenyl surface chemistry for designing scalable enzyme electrocatalysis and enzymatic fuel cells. I was introduced to this exciting and rapidly growing field of biological fuel cells by my postdoctoral advisor, Prof. Fraser Armstrong. Later, my own research group at Oklahoma State explored some aspects of the nanostructure-pyrenyl chemistry for enzyme bioelectrode designs. One of our current studies focuses on bucky paper-based biocathode designs with insights into direct electron transfer kinetics and electrocatalytic oxygen reduction to water. In summary, although the synthesis, optical, mechanical, and electronic properties of carbon nanomaterials are established, our understanding on the functioning of these materials in enzyme electrocatalysis is still at a primitive stage. As a result, the topic of nano-bioelectrocatalysis research has received a significant attention among electrochemists, who are now positioned to uncover the properties of these nanomaterials in an electrochemical environment.