Titanium carbide (Ti 3 C 2 T X ) MXene has prominent mechanical properties and electrical conductivity. However, fabricating high-performance macroscopic films is challenging, as weak interlayer interactions limit their mechanical performance. Here, we introduce [2]rotaxane, a mechanically interlocked molecule, to enhance MXene films. Compared to pure MXene (fracture strain: 4.6%, toughness: 0.6 MJ/m 3 ), [2]rotaxane-bridged MXene (RBM) films achieve record-high strain (20.0%) and toughness (11.9 MJ/m 3 ) with only 3.6% [2]rotaxane by weight. Additionally, RBM films endure 500 stretch cycles (0 to 15% strain) with stable and reversible resistance alterations, making them ideal for stretchable electrodes. Notably, RBM films enable stretchable electroluminescent devices with reliable operation under 20% elongation and customizable luminescent patterns. This innovative use of mechanically interlocked molecules to cross-link MXene platelets advances MXene films and other two-dimensional materials in stretchable electronics.