Facet Engineering Boosts Interfacial Compatibility of Inorganic‐Polymer Composites

The interfacial compatibility between inorganic particles and polymer is crucial for ensuring high performance of composites. Current efforts to improve interfacial compatibility preferentially rely on organic modification of inorganic particles, leading to their complex process, high costs, and short lifespans due to aging and decomposition of organic modifiers. However, the fabrication of inorganic particles free from organic modification that is highly compatible in polymer still remains a great challenge. Herein, a novel facet‐engineered inorganic particle that exhibit high compatibility with widely used polymer interface without organic modification is reported. Theoretical calculations and experimental results show that (020) and (102) facets of inorganic particles modulate local coordination environment of Ca atoms, which in turn regulate d‐orbital electron density of Ca atoms and electron transfer paths at interfaces between polymer and inorganic particles. This difference alters the molecular diffusion, orientation of molecular chains on surface of inorganic particles, further modulating interfacial compatibility of composites. Surprisingly, the facet‐engineered inorganic particles show exceptional mechanical properties, especially for tensile strain at break, which increases by 395%, far superior to state‐of‐the‐art composites counterparts. Thus, the method can offer a more benign approach to the general production of high‐performance and low‐cost polymer‐inorganic composites for diverse potential applications. The potential of utilizing facet engineering is effectively demonstrated to optimize the interfacial compatibility of IPCs without the use of organic modifiers. The findings revealed the distinctive electron transfer interactions between the (102) facet of AH and the PP molecules. It offers valuable insights into how facet engineering can selectively customize the mechanical properties of composites.