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In order to improve the dispersion and compatibility of the hydroxyl silicates (HNSs) in organic resin matrix, the HNSs were first functionalized by N‐(2‐aminoethyl)‐3‐aminopropyltrimethoxysilane (KH‐792) via a hydrolysis process; thus, the imino and amidogen groups can be grafted on the surface of HNSs (NH2‐HNSs). Fourier transform infrared spectroscopy, scanning electron microscopy, and X‐ray photoelectron spectroscopy are employed to characterize the chemical structure and surface morphology changes on the surface of HNSs after modified. The modified NH2‐HNSs were then used as fillers to add into bismaleimide (BMI) to prepare the new NH2‐HNSs/BMI composites. The influences of NH2‐HNSs content on the mechanical, tribological, and thermal properties of BMI resin were also researched. The results showed that adding NH2‐HNSs with appropriate content (6.0 wt%) could significantly improve the comprehensive properties of the NH2‐HNSs/BMI composites. It can be observed from the scanning electron microscopy (SEM) on the wear surface of the materials that, the wear mechanism of the BMI resin was converted from adhesive wear to abrasive wear after the addition of NH2‐HNSs. The improvement of tribological and mechanical properties can be mainly attributed to the chemical reaction between BMI and NH2‐HNSs. [ABSTRACT FROM AUTHOR]