To address the inherent challenge of functionalizing luminescent materials with record-high comprehensive self-healing performance and mechanical capacities, a spider-silk-inspired elastomer was synthesized by integrating hydrogen bonding (H-bonding) arrays together with lanthanide-bipyridine (abbreviated as Ln³⁺-Bpy) coordination bonds into polymer chains. The representative sample (denoted as APU-Bpy_0.1-Ln) shows an outstanding engineering tensile fracture strength of 38.34 ± 2.16 MPa, an engineering tensile strain of 2218 ± 15% and a superior toughness of 368.19 MJ m⁻³. The true fracture stress (0.89 GPa) of the APU-Bpy_0.1-Ln sample is comparable to that of the typical spider silk. Besides, the room-temperature self-healing performance of the resulting materials was achieved due to the dynamic abilities of the H-bonding arrays and lanthanide-bipyridine coordination bonds. The obtained APU-Bpy_0.1-Ln materials also exhibit multi-color emission and transparent and colorless behavior. We believe that this study provides a practically feasible strategy for the synthesis of luminescent/non-luminescent elastomers with self-healing abilities and superior comprehensive mechanical properties.