The amylose-water interaction is part of an important equilibrating process within the starch matrix leading to slow recrystallization of amylose chains and growth of anisotropic properties in the starch matrix. This article highlights the influence of nanoclay on (a) the structural development of amylose crystallinity and (b) the rate of water loss from the starch matrix. By varying the nanocomposites level (1.5-4 wt %), a unique microstructure is obtained that "locks" moisture and it was found that on a per unit weight basis of the starch matrix, addition of 4 wt % nanoclay resulted in additional 8.5% water in the matrix. Also, it was found that increasing the nanoclay from 2 to 4% by weight, the composite modulus jumped by 100% indicating excellent interaction between clay nanocomposites and starch polymer. Analysis of the starch crystallinity data indicates that nanocomposites retard the mobility of the starch molecules (specially the long chain amylose component) to restrict the movement of "associated" water around starch and this increases the "locked" water by similar to 10%. The results strongly suggest that a new structural unit may be formed by amylose-water-clay interaction which enhances the composites properties. (C) 2008 Wiley Periodicals, Inc.