A new magnetic polymer nanocomposite based on Fe 3 O 4 nanoparticles and nature rubber was prepared by the in situ latex method. This process was fast, versatile, reliable, safe, environmentally friendly, and inexpensive. The magnetorheological effect and mechanical properties of magnetic polymer nanocomposites were investigated in detail. The tensile strength of magnetic polymer nanocomposites without other reinforcing fillers was about 14.6 MPa. At the same time, the relative and absolute magnetorheological effect was about 365.0% and 3.64 MPa, respectively, which were almost 10 times with respect to other magnetic polymer nanocomposites based on nature rubber. Furthermore, the relationships between microstructure and mechanical behavior of magnetic polymer nanocomposites were simulated and discussed by the numerical treatment of a new theoretical model associated with finite element analysis for explaining the micro-mechanism of magnetic polymer nanocomposites with high performance. The work did not only provide a universal route for the rational design and preparation of magnetic polymer nanocomposites with simultaneously high magnetic sensitivity and mechanical properties for various applications but also propose a new method to improve dispersion of magnetic particles in nature rubber for various applications. KEYWORDS in situ latex, magnetorheological effect, magnetic polymer nanocomposites, mechanical properties, theoretical model