In this study, we have synthesized poly(1-NA-co-oT) and sphere-like NiCoO2 nanomaterials and then samples-with-layers were prepared to examine microwave absorption properties. For mono-layer, NiCoO2 exhibits superior microwave absorption capabilities than poly(1-NA-co-oT) sample. And for the bilayer sample, different samples were prepared with different layer thicknesses having poly(1-NA-co-oT) layer on top and NiCoO2 as base layer. The optimal bilayer sample having 1-mm thickness of each layer had excellent microwave absorption characteristics; indicating achieving a significant level of absorption necessitates a careful equilibrium between dielectric and magnetic loss. Additionally, best bilayer specimen has excellent absorption characteristics, as shown by its minimum reflection loss (RLmini) of −36 dB and effective absorption bandwidth of 3.5 GHz. Simulated and experimental findings of the bilayer optimal sample were compared and they were in accordance. The aforementioned results indicate a potential shift in the future creation of microwave-absorbing materials.