Abstract: | The mechanical properties of multiwall carbon nanotube (MWNT)/poly(methyl methacrylate) (PMMA) nanocomposites were studied as a function of nanotube orientation, length, concentration, and type. Orientation and dispersion were assessed by electron microscopy. A processing parameter study revealed the robust nature of fabricating nanotube/PMMA nanocomposites. An optimal set of extrusion conditions was found for minimizing the aggregate size in single‐wall carbon nanotube (SWNT)/PMMA nanocomposites; this set was also used for the fabrication of the MWNT/PMMA composites. Good dispersion was achieved for MWNTs in PMMA at 0.1–10 wt % loading levels (with the best dispersions at the lower loading levels). The orientation of MWNTs in PMMA proved to be the only way to substantially toughen the nanocomposite. A level of 1 wt % MWNTs in PMMA (oriented nanocomposite) exhibited the largest increase in tensile toughness with a 170% improvement over oriented PMMA. Increases in the modulus and yield strength were not nearly as pronounced (and occurred only at the highest loading of MWNTs, which was 10 wt %) with increases of 38 and 25%, respectively. A failure mechanism was proposed in which orientation of the MWNTs (normal to the direction of craze propagation and crack development) enabled them to toughen the brittle PMMA by bridging cracks that developed (via craze precursors) during the tensile test. None of the nanotube/PMMA composites showed mechanical properties close to the values expected from simple rule of mixture and orientation considerations. © 2004 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 42: 2690–2702, 2004 |