Carbon nanomaterials (CNMs) have been extensively used as electrochemical sensing composites due to their interesting chemical, electronic, and mechanical properties giving rise to increased performance. Due to these materials’ unknown long-term ecological fate, care must be given to make their use tractable. In this review, the design and use of carbon nanotubes (CNTs), graphene, and carbon dots (CDs) as electrochemical sensing electrocatalysts applied to the working electrode surface are surveyed for various biosensing applications. Graphene and CDs are readily biodegradable as compared to CNTs. Design elements for CNTs that carry over to graphene and CDs include Coulombic attraction of components and using O or N atoms that serve as tethering points for attaching electrocatalytically active nanoparticles (NPs) and/or other additives.