Metamaterials have surprisingly broadened the range of available practical applications in new devices such as shielding, microwave absorbing, and novel antennas. More research has been conducted related to tuning DNG frequency bands of ordered or disordered metamaterials, and far less research has focused on the importance of impedance matching behavior, with little effort and attention given to adjusting the magnitude of negative permittivity values. This is particularly important if devices deal with low-amplitude signals such as radio or TV antennas. The carbon/hafnium nickel oxide (C/Hf0.9Ni0.1Oy) nanocomposites with simultaneously negative permittivity and negative permeability, excellent metamaterial performance, and good impedance matching could become an efficient alternative for the ordered metamaterials in wave-transparent, microwave absorbing, and solar energy harvesting fields. In this study, we prepared C/Hf0.9Ni0.1Oy nanocomposites by the solvothermal method, and we clarified how the impedance matching and double-negative (DNG) behaviors of C/Hf0.9Ni0.1Oy can be tuned by an external AC electric field created by an electric quadrupole system. An external electric field allows for the alignment of the well-dispersed nanoparticles of carbon with long-range orientations order. We believe that this finding broadens our understanding of moderate conductive material-based random metamaterials (MCMRMs) and provides a novel strategy for replacing high-loss ordered or disordered metamaterials with MCMRMs.