High-performance sealants using rubber composites containing multiwalled carbon nanotubes (MWNTs) were developed in order to probe and excavate oil in deeper wells. However, the stress-strain behavior and the reinforcing mechanism of highly concentrated MWNT/rubber composites subjected to large deformation remain largely unexplored. Here we report on the complete stress-strain relationships of MWNT/rubber composites under uniaxial tension before rupture, with a suggestion of a novel reinforcement effect of high concentration of MWNTs. A theoretical model is developed to understand the reinforcing mechanism and estimate the mechanical properties of MWNT/rubber composites under large deformation. We have demonstrated that persistence length and reorientation of MWNTs during stretch have a significant impact on mechanical properties, such as the modulus of the rubber composite. These results provide guidelines for developing MWNT-reinforced composites to achieve desired nonlinear and extreme mechanical performance for a wide range of applications.