Graphene Oxide Capped Mechanically Interlocked Networks ^†

Comprehensive Summary Mechanically interlocked networks (MINs) provide a versatile platform for engineering materials that combine mechanical strength with dynamic adaptability. Their performance hinges on the constrained intramolecular motion of mechanical bonds, so the deliberate selection of capping groups is essential for tailoring properties. Herein, we develop an innovative capping strategy for mechanical bonds by employing graphene oxide (GO) as the capping unit, enabling the construction of a new class of mechanically interlocked networks ( GO MINs) with enhanced mechanical performance. GO MINs benefit both from the reinforcing effect of GO as a nanofiller and its innovative use as a capping unit that creates continuous mechanical bonds, collectively improving their mechanical strength and adaptability. Compared to the non‐interlocked control sample, GO MINs exhibit greater fracture strength (maximum stress: 9.4 vs. 3.6 MPa), higher toughness (22.3 vs. 9.7 MJ/m 3 ), and increased elongation at break (359% vs. 328%). Notably, despite these significant enhancements, GO MINs maintain good energy dissipation capacity and thermomechanical stability owing to the constrained intramolecular motion of mechanical bonds. This strategy endows GO MINs with distinctive properties, providing a promising platform for the design of advanced composite materials with enhanced and tunable multifunctionality.