Owing to its superb thermal and electrical attributes, as well as electrochemical stability, carbon is emerging as an attractive material for fabrication of many bioelectrochemical devices such as biosensors and biofuel cells. However, carbon’s inert nature makes it difficult to functionalize with biocatalysts; often requiring harsh chemical treatment, such as nitric acid oxidation, to attach reactive amines and carboxylic acids to its surface. Recent studies, however, points toward a self-assembly approach for fabricating well organized layers of carbon loaded with arrays of metallic nanoparticles patterned by block-copolymers (BCP) templates. Herein, we demonstrate an effective method for developing carbon nanofibers meshes embedded with metal nanoparticles, by incorporating a BCP self-assembly approach into our C-MEMS fabrication technique. The main phase of this hybrid method includes electrospinning metal salt-loaded BCP into nanofiber meshes, and subsequently reducing the metal salts into metal nanoparticles prior to pyrolysis. This cost-effective process will pave the way for fabricating scalable advanced 3-D carbon electrodes that can be applied to biosensors and biofuel cells devices.