The progress of advanced materials has invoked great interest in promising novel biosensing applications. Field-effect transistors (FETs) are excellent options for biosensing devices due to the variability of the utilized materials and the self-amplifying role of electrical signals. The focus on nanoelectronics and high-performance biosensors has also generated an increasing demand for easy fabrication methods, as well as for economical and revolutionary materials. One of the innovative materials used in biosensing applications is graphene, on account of its remarkable properties, such as high thermal and electrical conductivity, potent mechanical properties, and high surface area to immobilize the receptors in biosensors. Besides graphene, other competing graphene-derived materials (GDMs) have emerged in this field, with comparable properties and improved cost-efficiency and ease of fabrication. In this paper, a comparative experimental study is presented for the first time, for FETs having a channel fabricated from three different graphenic materials: single-layer graphene (SLG), graphene/graphite nanowalls (GNW), and bulk nanocrystalline graphite (bulk-NCG). The devices are investigated by scanning electron microscopy (SEM), Raman spectroscopy, andI-Vmeasurements. An increased electrical conductance is observed for the bulk-NCG-based FET, despite its higher defect density, the channel displaying a transconductance of up to ≊4.9×10−3A V−1, and a charge carrier mobility of ≊2.86×10−4cm2V−1s−1, at a source-drain potential of 3 V. An improvement in sensitivity due to Au nanoparticle functionalization is also acknowledged, with an increase of the ON/OFF current ratio of over four times, from ≊178.95to ≊746.43, for the bulk-NCG FETs.