Nanocomposites were prepared by melt mixing ethylene/methacrylic acid copolymers and organoclays, which were compared to equivalent composites prepared from low-density polyethylene (LDPE) and a sodium ionomer of poly(ethylene-co-methacrylic acid). The effects of matrix modification and organoclay structure on the morphology and properties of these nanocomposites were evaluated using stress-strain analysis, wide-angle X-ray scattering (WAXS), and transmission electron microscopy coupled with particle analysis. With all four polymers, the use of a two-tailed organoclay, M-2(HT)(2), led to the formation of more exfoliated nanocomposites than a one-tailed organoclay, M-3(HT)(1). Nanocomposites prepared from ethylene/methacrylic acid copolymers revealed better exfoliation compared to similar composites prepared from LDPE. It seems that the presence of relatively small quantities (1.3-3.1 mol%) of the polar methacrylic acid monomer aids in improving the organoclay exfoliation efficiency of these polymers. Nanocomposites prepared from the sodium ionomer of poly(ethylene-co-methacrylic acid) exhibited the highest levels of organoclay exfoliation compared to all other polymers examined in this study. However, from the observations made in this study, it was not possible to determine conclusively the relative interaction of carboxyl acid groups versus the salt form with the organoclay and, thus, their influence on exfoliation; additional studies will be needed to reach a conclusion on this important point. (c) 2007 Elsevier Ltd. All rights reserved.