Low-voltage, organic field-effect transistors (OFETs) have a high potential to be key components of low-cost, flexible, and large-area electronics. However, to be able to employ OFETs in the next generation of the electronic devices, the reduction of their operational voltage is urgently needed. Ideally, to be power efficient, OFETs are operated with gate voltages as low as possible. To fulfill this requirement, low values of transistor threshold voltage (Vt) and subthreshold swing (SS) are essential. Ideally, Vt should be around 0 V and SS close to 60 mV/dec, which is the theoretical limit of subthreshold swing at 300 K. This is a very challenging task as it requires the gate dielectric thickness to be reduced below 10 nm. Here, the most promising strategies toward high capacitance dielectrics for low voltage operated OFETs are covered and discussed.