This work reports on a novel magnetorheological polymer gel with carbon nanotubes and carbonyl iron particles mixed into the physical cross-linked polymer gel matrix. The resulting composites show unusual nonlinear magneto-electro-mechanical responses. Because of the low matrix viscosity, effective conductive paths formed by the CNTs were mobile and high-performance sensing characteristics were observed. In particular, due to the transient and mutable physical cross-linked bonds in the polymer gel, the electromechanical behavior acted in a rate-dependent manner. External stimulus at a high rate significantly enhanced the electrical resistance response during mechanical deformation. Meanwhile, the rheological properties were regulated by the external magnetic field when magnetic particles were added. This dual enhancement mechanism further contributes to the active control of electromechanical performance. These polymer composites could be adopted as electromechanical sensitive sensors to measure impact and vibration under different frequencies. There is great potential for this magnetorheological polymer gel in the application of intelligent vibration controls.