The structure-property relationship of polymer/layered silicate nanocomposites was investigated in this study. Polymer nanocomposites based on completely amorphous poly(hexamethylene isophthalamide) with exfoliated, intercalated, or agglomerated nanoclay morphology were produced and analyzed by X-ray diffraction and transmission electron microscopy. Differential scanning calorimetry measurements were used to characterize the glass-transition behavior. Dynamic mechanical analysis was performed to investigate the nature of the constrained region as the reinforcement mechanism. The modulus enhancement of the organoclay nanocomposites was found to have good linear correlation with the volume of the constrained region. The type of polymer-nanofiller interaction strongly influences the amount and modulus of the constrained region, and both of the latter contribute to the enhancement in the storage modulus of the polymer nanocomposite. The mechanical properties of the constrained region are temperature-dependent. Constrained region models for polymer nanocomposites were proposed on the basis of these results. The constrained volume in amorphous polymer nanocomposites was found to be much less than that in semicrystalline systems.