Multi-/many-core, homogeneous or heterogeneous architectures, using the existing CMOS technology are inevitably approaching the limit of attainable power efficiency due to the fundamental limits in scaling. Negative Capacitance Field-Effect Transistor (NCFET) is rapidly emerging as an alternative technology that promises a multi-fold increase in the power efficiency of transistors, yet is compatible with the existing CMOS fabrication process. NCFET incorporates a ferroelectric (FE) layer within the transistor’s gate stack, which exhibits a negative capacitance effect amplifying the internal voltage. NCFET has been in detail studied in both physics and devices/circuits communities where its superiority has been demonstrated in semiconductor measurements. However, the full promise of NCFET remains unmodeled and unquantified unless the research is further continued to the microarchitecture and system levels. This article, for the first time, explores system- and application-level benefits of NCFET-based multi-/many-core designs in terms of performance and power-efficiency compared to state-of-the-art FinFET-based designs. This exploration is done first through analytical modeling in which we extend Amdahl’s law for NCFET multi-/many-cores, and then through quantitative modeling. The latter is achieved through RTL- and system-level simulations of NCFET-based multi-cores. The analytical modeling shows that a novel type of technology-based heterogeneity in which cores with the same microarchitecture but different FE thickness are combined is highly beneficial. Our exploration shows that this novel heterogeneity increases the power-efficiency by up to 3.5× over homogeneous systems and even achieves 8.3% better performance and 20% higher power-efficiency than conventional heterogeneity in the microarchitecture without having to cope with the complexity of managing different microarchitectures.