Sub-micron thick flakes were obtained by sonication of vermiculite that was first exfoliated by either thermal shock or chemical treatment with hydrogen peroxide. Dimer fatty acid polyamide nanocomposites with a mixed morphology were prepared via a solution-dispersion technique. The large (in the micrometer range) vermiculite flakes assumed random orientations in the matrix. BET surface area measurements indicated flake thickness below 100 nm but SEM showed that thicker flakes were also present. Filler content was varied up to 30 wt.%. At this loading, the tensile strength doubled, the modulus increased five-fold but the elongation-at-break decreased by a factor of ten. Dynamic mechanical analysis suggests three stiffening mechanisms. The reinforcing effect of the high stiffness inorganic flakes is the primary contributor. Together with the chain confinement effect, that expresses itself in an apparent increase in the glass transition temperature, provides an adequate rationalisation of the stiffness variation below Tg. However, an additional stiffening effect is indicated at temperatures above Tg. The mechanism may involve dynamic network formation based on fluctuating hydrogen bonding interactions between the matrix polymer chains and the filler particles.