A novel multifunctional composite material, defined as self-healing magnetorheological elastomer (SH-MRE), which exhibits both shear stiffening and magnetorheological effects as well as self-healing ability, is obtained by dispersing carbonyl iron particles in a poly(urethane-urea) matrix. The dynamic shear properties are tested through oscillation frequency and magnetic field sweeps. When shear stress is applied with an excitation frequency of 0.1 Hz to 100 Hz, the storage modulus of the poly(urethane-urea) matrix increases sharply, showing a good shear stiffening effect. In addition to the magnetically dependent mechanical properties with a magnetic flux density of 0–0.894 T, the self-healing efficiency of the isotropic SH-MREs with destructive shear damage after healing can be influenced by the mass fraction of the carbonyl iron particles, the applied magnetic field strength and the support of trace solvents. Based on the experimental results, it is believed that the hydrogen bonds in the dynamic hard domains and the magnetic interaction forces between the carbonyl iron particles induced by the magnetic field are the cause of the good multifunctional properties.
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