Metal nanoparticles have been widely used for many catalytic and electrocatalytic applications due to their larger surface area-to-volume ratios and higher densities of active sites compared to bulk materials. This has resulted in much interest in understanding the electrocatalytic behavior of metal nanoparticles with respect to their structure. However, most research on this topic has employed collections of nanoparticles. Due to difficulties in controlling and characterizing particle loading and interparticle distance in nanoparticle ensembles, single nanoparticles studies have recently become a topic of great interest. In this study, a soft nitriding technique was applied to chemical vapor-deposited carbon ultramicroelectrodes (UMEs) in order to immobilize ligand-free AuNPs onto the carbon substrate. The feasibility of this method is geared toward studying the properties of single AuNPs immobilized onto carbon nanoelectrodes. The ligand-free AuNPs immobilized onto the nitrided carbon UMEs were highly electrocatalytic toward methanol oxidation.