Metacomposites with negative electromagnetic properties are promising candidates for thin-film capacitors, wearable cloaks, and electromagnetic wave attenuation. In contrast to the complicated preparation procedures of traditional structural metamaterials, a two-dimensional (2D) polypyrrole nanoring (PPy NR) was constructed employing a facile soft template method. Negative permittivity and negative magnetic susceptibility were simultaneously observed in two-dimensional PPy loop structure and carbon nanotube (MWCNT)/PPy NR multi-dimensional composite materials, these properties exhibited significant dependence on the microstructures. The two-dimensional loop structure that contributed to the negative magnetic susceptibility could be conveniently adjusted through the morphology of the soft template. The conductive networks formed by PPy NRs and MWCNTs appeared to promote the apparent negative permittivity as well as negative electromagnetic properties within 100 MHz-1 GHz. The study of the structural design not only provided a novel approach for the realization of negative permittivity, but also offered a new design paradigm for negative magnetic susceptibility metacomposites. • PPy NRs with 2D loop-shaped microstructure were constructed employing a facile soft template method. • The 2D loop structure was conducive to the generation of negative permittivity and negative magnetic susceptibility due to their innate character of possessing many conductive loops. • Simultaneous negative permittivity and negative magnetic susceptibility properties were observed.