This study presents carbon attachment on an aluminum nitride (AlN) gate dielectric to improve the device performance of pentacene-based organic thin-film transistors (OTFTs). This approach produces high OTFT performance on an aged AlN surface. A high mobility of 0.67 cm2 /V s was achieved on an AlN surface aged for 14 days, compared to a mobility of 0.05 cm2 /V s on an as-deposited AlN surface. This improvement in device performance is correlated with carbon attachment on the AlN surface, which lowers surface energy. The lowered surface energy made the surface less polar, as measured by a contact angle instrument. The chemical composition of the aged AlN surface was analyzed using x-ray photoelectron spectroscopy before pentacene deposition. Enhanced C=C bonding at 284.5 eV was observed on the aged AlN surface. These enhanced C=C bonds favored the growth of large pentacene islands in the initial growth stage, which may improve OTFT device performance.