negative-capacitance (NC) effect [3] has recently attracted much attention. [4][5][6][7] NC-FETs incorporate ferroelectric (FE) on dielectric (DE) layers, [8][9][10][11][12][13][14][15][16][17][18] but they are obviously different from FE-gated or highk DE-gated transistors (as categorized in Table S1 in the Supporting Information). For NC-FETs, their operation relies on the anomalous polarization response of FE gate material to the external electric field. Although other types of novel FETs such as topological quantum FET, [19] tunnel FETs, [20,21] and impact ionization MOSFETs [22] have also been proposed as alternatives to overcome the same challenge, NC-FET has great advantages in its simplicity for device fabrication over the other FETs. Despite its great potential for reducing SS, NC-FETs usually exhibit hysteresis during operation, which is detrimental to logic device applications. The hysteresis originates from the bistable polarization configuration of the FE gate insulator. (FE-gated FET shows large hysteresis with low SS, while high-k DE-gate FET shows little hysteresis but a relatively large SS.) Recently, researchers have found that the proper capacitance matching between DE and FE layers can ensure the hysteresis-free device operation. [7,[23][24][25] However, the FE/DE capacitance matching is only feasible via a precise thickness control of FE and DE layers, which is often very difficult to achieve. Therefore, even with significant engineering efforts, the realization of hysteresis-free NC-FET with reduced SS has been challenging. Most of the Negative-capacitance field-effect transistors (NC-FETs) have gathered enormous interest as a way to reduce subthreshold swing (SS) and overcome the issue of power dissipation in modern integrated circuits. For stable NC behavior at low operating voltages, the development of ultrathin ferroelectrics (FE), which are compatible with the industrial process, is of great interest. Here, a new scalable ultrathin ferroelectric polymer layer is developed based on trichloromethyl (CCl 3 )-terminated poly(vinylidene difluoride-cotrifloroethylene) (P(VDF-TrFE)) to achieve the state-of-the-art performance of NC-FETs. The crystalline phase of 5-10 nm ultrathin P(VDF-TrFE) is prepared on AlO X by a newly developed brush method, which enables an FE/dielectric (DE) bilayer. FE/DE thickness ratios are then systematically tuned at ease to achieve ideal capacitance matching. NC-FETs with optimized FE/DE thickness at a thickness limit demonstrate hysteresis-free operation with an SS of 28 mV dec −1 at ≈1.5 V, which competes with the best reports. This P(VDF-TrFE)-brush layer can be broadly adapted to NC-FETs, opening an exciting avenue for low-power devices.