||To provide a better understanding of the relationship between nanostructure and overall material stiffness in the case of polymer/clay nanocomposites, both analytical and finite element modeling were considered. A micromechanical analytical approach based on a multiscale framework is presented in which special attention is devoted to the constrained region around reinforcements. The thickness of the constrained region is seen as a characteristic length scale and the effect of particle size is explicitly introduced in the model. Moreover, the constrained region presents graded properties. The hierarchical morphology of intercalated silicate stacks is also explicitly introduced in the micromechanical model from an equivalent stiffness method in which the silicate stacks are replaced by homogeneous particles with constructed equivalent anisotropic stiffness. The orientational averaging process is used to derive the overall stiffness tensor of nanocomposite materials containing randomly oriented reinforcements. The respective influence of volume fraction, aspect ratio, size and orientation of the reinforcements, matrix properties, number of silicate layers per stack, and interlayer spacing on the overall nanocomposite stiffness is analyzed. The overall stiffness of polymer/clay nanocomposite systems is also evaluated by means of finite element simulations and the results compare favorably with model predictions. From an experimental point of view, relevant morphological and mechanical data were obtained on polyamide-6 nanocomposites prepared using a modified montmorillonite Cloisite 30B and an unmodified sodium montmorillonite Cloisite Na+. The amount of constrained region around reinforcements was estimated using results issued from dynamic mechanical analyses and differential scanning calorimetry. Comparison to the model clearly underlines the contribution of the constrained region to the stiffness improvement.