In this work, a series of nanoporous carbon materials were synthesized using Iranian asphalteneas a low-cost carbon source and modified by melamine as a new nitrogen-rich promoter(M-IANC).The adsorption capacity ofbenzene and toluene on the synthesized M-IANCs was measured at low and high concentrations by an in-house built apparatus. The results demonstrated that the addition of melamine remarkably increased the mesoporous volume (up to 1.61 cm3/g) in the nanoporous carbon structure and, subsequently, created a large surface area (2692 m2/g) and pore volume (1.71cm3/g).The resulting M-IANC-C nanostructure (melamine:PIA mass ratio of 1:2) depicted 228.18 wt.% and 82.08 wt.% adsorption capacity for benzene and toluene, respectively, which were 19.4 and 2.8 times higher than commercial activated carbon. In addition to the distinguished adsorptive behavior for benzene and toluene removal, M-IANC-Cexhibited higher cyclic adsorption capacity than those of unmodified IANC sample after four consecutive cycles. The adsorption mechanism and the role of melamine groups in the adsorption of benzene and toluene were also studied by the density functional theory (DFT) calculations.Besides the inexpensive cost of the carbon source (asphaltene), results also indicate that the M-IANC can be a suitable candidate for VOC adsorption.