Facilely Synthesis of MOF-Derived Nickel Phyllosilicate Nanosheet Assembly and Its Application in Robust, Toughened and Wear-Resistant Epoxy Composites

Epoxy (EP) exhibits inherent brittleness and poor wear resistance, limiting its service under long-term frictional conditions. Two-dimensional layered nanofillers are promising candidates for tribological enhancement, yet uniform filler dispersion and robust filler–matrix bonding remain challenging. In this study, nickel phyllosilicate nanosheet assemblies (NiPS−NA) were synthesized via a two-step hydrothermal route using Ni-MOF as a sacrificial template and blended into the EP matrix to fabricate composites. A series of characterizations were carried out to evaluate the structure–property relationships of EP/NiPS–NA composites. Loosely stacked NiPS–NA nanosheets disperse uniformly within the EP matrix and comprehensively improve the comprehensive properties of EP/NiPS–NA composites. As NiPS–NA loading increases, elongation at break rises to a peak value of 6.0% at 3% filler content, representing a 43.3% improvement over neat EP, whereas tensile strength increases steadily with only minor variations in elastic modulus. Incorporated NiPS–NA suppresses thermal weight loss, elevates the high-temperature char yield and raises the activation energy for thermal decomposition. Notably, the composite containing 5% NiPS–NA delivers the lowest wear rate of 1.02 × 10−5 mm3/N·m, an 89.4% reduction relative to unfilled EP. Extensive examinations of worn surfaces further clarify the NiPS–NA-mediated wear mechanism. This work offers a facile three-in-one strategy for preparing high-performance wear-resistant polymeric composites.