Within the quantum-mechanical (QM) study, namely, atomistic simulations from the first principles we discussed structural, energetic and mechanical properties of the composite interfacial layers consisting of polymer component of the elastomeric rubber and amorphous carbon nanoparticles. In computer simulations the ways of the surface modifying of amorphous carbon particles that reduce the aggregation of filler particles and improve the physical and mechanical properties of the compositions as a whole have been defined. Sorption and chemical modifications of the surface of the filler particles are considered. A number of disaggregating dispersive media, in particular solvents, whose presence hinder aggregation of carbon filler particles and facilitate their dispersion in the polymer matrix, was examined. The modification of the surface of carbon particles was considered with formation of covalent bonds with different surface-active groups. It was shown that such the chemical modification complicates the aggregation of filler particles, and greatly improves the mechanical and strength properties of the interfacial layer between the polymeric matrix and filler particles. It was found that chemical modification of the carbon particles is much more efficient than sorption modification. On the basis of this quantum-mechanical modeling the recommendations are given on the use and modification of carbon fillers of elastomeric rubbers.