attention. Typically, researchers focus on achieving this unique property through the specially designed array units. Afterward, it was discovered that the extraordinary properties can also be obtained from materials with specific components. These metamaterials are called intrinsic metamaterials or metacomposites. [4] Moreover, compared with traditional metamaterials, metacomposites have some advantages such as their size could be simply changed while the size of traditional metamaterials depends on the wavelength of the applied electromagnetic field. So it is possible to prepare ultrathin and isotropic intrinsic metamaterials. [5] There are two ways to generate negative permittivity and negative permeability, respectively. First, two different types of negative permittivity, dipole-type and plasma-type, [6] were observed in composites. The plasma-type negative permittivity is ascribed to low frequency plasmonic state that is generated from the conductive networks, [7] which could be explained by Drude model. However, the resonance-induced electric dipole negative permittivity is generated from isolated conducting particles, which could be explained by Lorentz model. Specifically, when the amount of functional filler in the composite reaches a critical value, the filler particles directly come into contact with each other, forming a continuous network structure in the whole system and the percolating phenomenon appears. [8] As the microstructure of materials change, the physical properties of them also undergo an abrupt shift and bring about unique properties, such as high dielectric constant or high electrical and thermal conductivity. It is worth noting that researchers discovered the negative permittivity could be obtained when the functional filler exceeds the percolation threshold, which is consistent with the Drude model theoretically. Accordingly, it offers an effective way for the design of intrinsic metamaterial. Various types of conductive fillers including metal fillers, [9] carbon materials, [10] and conductive polymers [11] are used to fabricate metacomposites with negative dielectric constant. There are also some researchers construct metamaterials with negative permittivity following the Lorentz model. [12,13] There are also two completely different mechanisms for the generation of negative permeability. In one case, the negative parameter is ascribed to magnetic particles in composite.Metacomposites have received significant interest over the past decade due to their unique double-negative electromagnetic properties. Magnetic particles, conductive polymer, and carbon materials are the usual materals used to fabricate metamaterials with doube-negative electromagnetic properties. Here, insulating polymer polyolefin elastomer is instead used as the matrix to construct such metacomposites. The composites are fabricated by using a swelling, bonding, and hot pressing process. Metacomposites in which 50 vol% binder and 3 vol%, 6 vol%, and 12 vol% multi-walled carbon nanotubes are added show negative per...