5376 wileyonlinelibrary.com traditional dielectrics and semiconductors in organic fi eld-effect transistors (OFETs). For example, the development of hybrid dielectrics, which are comprised of an ultrathin high-k metal oxide layer in conjunction with an SAM, enables low-voltage high-performance operation of organic transistors. [16][17][18] Self-assembled monolayer fi eld-effect transistors (SAMFETs) are a promising concept that uses rationally designed π-conjugated SAMs as the semiconductor of a transistor. [19][20][21][22][23] This concept works in principle because charge transport in an organic semiconductor-based FET occurs in the fi rst few monolayers closest to the dielectric. [ 24,25 ] SAMFETs are believed to have a broad appeal for organic semiconductor device applications due to their low-cost processing, reduced material quantity needed compared to tradition organic thin fi lm transistors, and ability to be used toward fl exible electronics and sensing applications. Signifi cant progress has been made through molecular design and novel device architecture to achieve a state-of-the-art hole mobility of around 10 −2 cm 2 V −1 s −1 . In order to achieve further performance enhancement, it is critical to overcome a fundamental challenge of effi cient contact between the metal source/drain electrodes and SAM semiconductor in SAMFET devices. Effi cient contacts between SAM semiconductor and electrodes may have been enabled by Smits et al. through under-etching the electrodes allowing the SAM to form underneath or, as shown by Schmaltz et al. , through utilizing a secondary SAM to elevate the electrodes to allow edge-on contact with the SAM semiconductor core. [ 20,21 ] However, these reports utilize cumbersome and complicated device architectures that may make SAMFETs less appealing toward commercialization. Furthermore, little work has been done to examine the impact of SAM processing on molecular packing density.Herein we demonstrate top-contact bottom-gate low-voltage p-type SAMFETs with a hybrid hafnium oxide (HfO 2 ) dielectric that operates under a bias of −3 V and has a charge carrier mobility of 10 −2 cm 2 V −1 s −1 . Charge carrier mobility of the SAMFET is increased by over two orders of magnitude through the designed functional SAM terminal group that enables effi cient charge injection between metal electrode and SAM