The suitability of metal‐organic frameworks (MOFs) as functional materials for future electronic logic devices with desirable dielectric constant, bandgap, high‐quality interface, low leakage current, and better compatibility is still an open challenge. Owing to the synergistic complementary properties of MOFs systems, a low‐cost copper‐metal‐organic nanoclusters (Cu‐MOCs) has been synthesized comprising inorganic copper metal unit allied organic m‐toluic acid ligand by facile sol–gel strategy. It offers large‐area thin‐films uniformity, high dielectric constant (κ ≈ 5.49), improved interfacial properties, dynamic switching behavior with the stimuli field, and extends the realization of metal‐organic‐framework dielectric for scalable complementary‐metal‐oxide‐semiconductor (CMOS) logic applications over customary hybrid counterparts. Various techniques such as single crystal X‐ray diffraction, X‐ray photoelectron spectroscopy, thermogravimetric analysis, and energy dispersive X‐ray spectroscopy have been used to validate the Cu‐MOCs formulation. In particular, the fabricated Cu‐MOCs, metal–insulator–semiconductor structures exhibit promising dynamic switching behavior responsive to the applied field, hysteresis‐free capacitance–voltage characteristics, low interfacial trap density (≈1.4 × 1011 eV−1 cm−2), low effective oxide charges (≈1.1 × 1011 cm−2), and noteworthy small leakage current density (≈1.29 nA cm−2 @ 1 V) ever since in electrical analysis. Cost‐effective novel Cu‐MOCs successfully demonstrate high‐performance, reliable gate dielectrics for next‐generation CMOS logic devices.