AbstractTo improve the subpar lubricating performance of epoxy resin, this paper presents the preparation of a novel bimetallic phyllosilicate featuring a distinctive rice‐granular morphology, which incorporates nickel and iron metal cations through a facile hydrothermal process. These phyllosilicates were then integrated into the epoxy matrix to form composites. A comprehensive analysis of the target product validates the rationality of the synthesis strategy for the as‐prepared rice‐granular bimetallic nickel/iron phyllosilicate, demonstrating a homogeneous hierarchical structure with numerous tiny nanosheets of nickel/iron phyllosilicate grown in situ on the flat surfaces of the rice‐granular metal–organic frameworks. An adequate addition of nickel/iron phyllosilicates allows for excellent dispersion within the matrix and establishes strongly bonded interfaces, steadily increasing the elastic modulus and hardness. Notably, the average friction coefficients decrease from 0.515 for the pure resin to 0.450 for the composites when the filler content reaches 7%, indicating a significant solid lubrication effect. In contrast, adding just 1% nickel/iron phyllosilicate moderately improves wear resistance, elongation at break, and tensile strength. Furthermore, it was found that as the filler content increased, the weight loss rate was reduced by approximately 43.8%, while the residual char increased by 74.2%, significantly enhancing the thermal stability of epoxy composites at high temperatures. This study offers a promising approach to preparing self‐lubricated epoxy composites with favorable mechanical and thermal properties.Highlights NiFePS was successfully synthesized via a facile two‐step self‐polymerization. Excellent mechanical properties of composites could be achieved with low content of NiFePS. The friction coefficient and wear rate were lowered remarkably. The friction mechanism was solid lubrication.