The combination of multiple physical properties is of great importance for widening the application scenarios of biomaterials. It remains a great challenge to fabricate biomolecules-based fibers gaining both mechanical strength and toughness which are comparable to natural spider dragline silks. Here, by mimicking the structure of dragline silks, a high-performance fluorescent fiber Alg-TPEA-PEG is designed by non-covalently cross-linking the polysaccharide chains of alginate with AIEgen-based surfactant molecules as the flexible contact points. The non-covalent cross-linking network provides sufficient energy-dissipating slippage between polysaccharide chains, leading to Alg-TPEA-PEG with highly improved mechanical performances from the plastic strain stage. By successfully transferring the extraordinary mechanical performances of polysaccharide chains to macroscopic fibers, Alg-TPEA-PEG exhibits an outstanding breaking strength of 1.27 GPa, Young's modulus of 34.13 GPa, and toughness of 150.48 MJ m