In this study, composites based on a thermoset polyurethane elastomer (PU) and multiwalled carbon nanotubes (MWCNT) in the case of a PU of high elastic modulus (>200 MPa) are analyzed for the first time. As-grown and modified nanotubes with 4 wt % of oxygenated functions (MWCNT-ox) were employed to compare their effect on composite properties and maxima mechanical properties (elastic modulus and tensile strength) were reached at 0.5 wt % of MWCNT-ox. Furthermore, by examining the morphology using optical and electron microscopies better dispersion and interaction of the nanotube-matrix was observed for this material. DMTA data supports the observation of an increase in the glass transition temperature of 20 C in the nanocomposites compared with the thermoset PU, which is an important result because it shows extended reliability in extreme environments. Finally, nanoindentation tests allowed a comparison with the conventional mechanical tests by measuring the elastic modulus and hardness at the subsurface of PU and the nanocomposites.