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Coil–rod copolymers with a dendritic polyethylene (DPE) core and multiple helical poly(γ-benzyl-L-glutamate) (PBLG) arms (DPE-(PBLG)_n) were prepared by palladium-catalyzed copolymerization in tandem with ring-opening polymerization (ROP). Macroinitiator (DPE–(NH₂)₁₁) was firstly prepared by the group transformation of DPE–(OH)₁₁ generated from palladium-catalyzed copolymerization of ethylene and acrylate comonomer. Coil–helical DPE-(PBLG)₁₁ copolymers were prepared by ROP of γ-benzyl-L-glutamate-N-carboxyanhydride (BLG-NCA). These DPE-(PBLG)₁₁ copolymers could form thermoreversible gels in toluene solvent, and the dendritic topology of the DPE core increased the critical gelation concentrations. The self-assembled nanostructure of gels was fully characterized by transmission electron microscopy (TEM), atomic force microscopy (AFM), small-angle X-ray scattering (SAXS), and wide-angle X-ray diffraction (WAXD), and the morphology of the fibrous structure was a twisted flat ribbon through a self-assembled nanoribbon mechanism. The self-assembled fibers formed by DPE-(PBLG₄₅)₁₁ are more heterogeneous and ramified than previously observed fibers formed by PBLG homopolymer and block copolymers.