Carbon nanomaterials are used to improve electrodes for neurotransmitter detection, but what properties are important for maximizing those effects? In this work, we compare a newer form of graphene, carbon nanospikes (CNSs), with carbon nanotubes (CNTs) grown on wires and carbon fibers (CFs). CNS electrodes have a short, dense, defect-filled surface that produces remarkable electrochemical properties, much better than CNTs or CFs. The CNS surface roughness is 5.5 times greater than glassy carbon, while CNTs enhance roughness only 1.8-fold. D/G ratios are higher for CNS electrodes than CNT electrodes, an indication of more defect sites. For cyclic voltammetry of dopamine and ferricyanide, CNSs have both higher currents and smaller ΔEp values than CNTs and CFs. CNS electrodes also have a very low resistance to charge transfer. With fast-scan cyclic voltammetry (FSCV), CNS electrodes have enhanced current density for dopamine and cationic neurotransmitters due to increased adsorption to edge plane sites. This study establishes that not all carbon nanomaterials are equally advantageous for dopamine electrochemistry, but that short, dense nanomaterials that add defect sites provide improved current and electron transfer. CNSs are simple to mass fabricate on a variety of substrates and thus could be a favorable material for neurotransmitter sensing.