The evolution of paramagnetic properties of the fullerene soot (FS), fullerene black (FB), and their polymer composites Phenylon C-2/FS, FB has been studied using the electron paramagnetic resonance (EPR) method. For the first time, a drastic growth of the EPR signals in the FB, FS, and composite samples was observed under pumping out at temperatures T = 20 ÷ 300 °C, which is attributed to the interaction between carbon defects and adsorbed gas molecules, mainly oxygen.It is shown that the ensemble of paramagnetic centers in the FB, FS, and the composite is heterogeneous. This ensemble consists of three spin subsystems 1, 2, and 3 related with different structural elements. The subsystems give three corresponding contributions, L
1, L
2 and L
3, into the overall contour of the EPR signal. The most intensive and broad signal L
3 is caused by 2D electrons from the surface of carbon flakes. Theoretical calculations of the L
3 signal line shape were carried out, and the decay rate of the integral intensity has been obtained for each component L
1, L
2, and L
3 after the contact of the sample with the ambient air. The signal decay process in the bulk composite samples is much slower due to their low gas permeability at room temperature (RT).