Here, we provide evidence that functionalizing the carbon-fiber surface with amines significantly improves direct electrochemical adenosine triphosphate (ATP) detection with fast-scan cyclic voltammetry (FSCV). ATP is an important extracellular signaling molecule throughout the body and can function as a neurotransmitter in the brain. Several methods have been developed over the years to monitor and quantitate ATP signaling in cells and tissues; however, many of them are limited in temporal resolution or are not capable of measuring ATP directly. FSCV at carbon-fiber microelectrodes is a widely used technique to measure neurotransmitters in real-time. Many electrode treatments have been developed to study the interaction of cationic compounds like dopamine at the carbon surface yet studies investigating how to improve anionic compounds, like ATP, at the carbon fiber surface are lacking. In this work, carbon-fibers were treated with N-(3-dimethylaminopropyl)-N'-ethylcarbodiimide (EDC) which reacts with carboxylic acid groups on the carbon surface followed by reaction with ethylenediamine (EDA) to produce NH2-functionalized carbon surfaces. Overall, we a 5.2 ± 2.5-fold increase in ATP current with an approximately 9-fold increase in amine functionality, as analyzed by X-ray Photoelectron Spectroscopy, on the carbon surface was observed after modification with EDC-EDA. This provides evidence that amine-rich surfaces improve interactions with ATP on the surface. This study provides a detailed analysis of ATP interaction at carbon surfaces and ultimately a method to improve direct and rapid neurological ATP detection in the future.