This study investigated the effects of intercalation and exfoliation of the graphite flake particles on the mechanical properties of elastomeric composites using analytical, computational, and experimental techniques. Relying on the modified Eshelby and incremental Mori–Tanaka approach, a new micromechanics model was proposed to estimate Young’s modulus and develop a constitutive model for expanded graphite (EG)-filled elastomer in finite strain deformation. It was found that when the initial graphite flakes expanded, the actual volume fraction and ultimate aspect ratio of the dispersed particles significantly affected the mechanical properties of the EG-reinforced composites. The present model and subsequent predictions reflect the initial flake diameter, actual volume fraction, ultimate aspect ratio of the particles, and other convenient physical properties of the composite constituents. In addition, molecular dynamics simulations were performed to evaluate the elastic properties of the EG-Matrix interphase region using the COMPASS force field function. The MD results showed that Young’s modulus of the interphase region increased significantly as the quantity of the graphene layer increased. The micromechanics-constitutive model results were validated using the experimentally determined stress–strain relation of the composites. EG- and CB-elastomer nanocomposite specimens were fabricated and tested in the experimental program. Field emission scanning electron microscopy (FESEM) analysis of the cryo-fractured surfaces of the elastomer compounds showed good interactions between the constituents. Numerical computations indicated that the proposed model incorporating the new parameters could accurately predict the experiment at a small particle concentration.