This article reports a bioinspired strategy for the preparation of robust soy protein isolate (SPI) based nanocomposites using a poly(dopamine) coating montmorillonite (D-MMT) as reinforcement and ferric ion (Fe (III) ) as a coordination crosslinking center. Typically, the catechol groups present on MMT provide multiple cross-linking reaction sites for bio-nanocomposites reinforcement: Coordination among Fe (III) -catechol interactions as well as covalent interactions based on the Michael addition/ Schiff base reaction or hydrogen-bonded between D-MMT and the SPI matrix. The morphological, mechanical, hydrophobic, water-resistant, and thermal behaviors of the resultant SPI-based nanocomposites were investigated. The interaction between D-MMT and the SPI matrix was investigated via the scanning electron microscopy and atomic force microscopy. The results showed that, with 5 wt% D-MMT loading, the tensile strength, and elasticity modulus of the SPI-based nanocomposite films increased by 75.2 and 135.2%, respectively, compared with the control. The enhanced mechanical properties of the obtained modified films were, in fact, a result of the multiple cross-linking system, as confirmed by the Fourier transform infrared spectroscopy and solid-state 13