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A high-performance anode material of Li-ion batteries, CNTs@MoS2 hybrid, was rationally designed and synthesized through a novel polyelectrolytes-based approach. Thanks to the spatially controlled effect of LBL self-assembled three-layered polyelectrolytes(PDDA/PSS/PDDA),ultrathin 2D MoS2 nanosheets with highly exposed edge sites are homogenously grown on the surface of 1D CNTs. Benefiting from this unique structure, CNTs@MoS2 hybrid manifests excellent rate behavior and cycling stability as anode material of Li-ion batteries. In addition. this approach is found effective in the growth of 2D MoS2 nanosheets on the other two types of 1D CNFs, demonstrating its universal applicability to the growth of MoS2 on various carbon substrates irrespective of the surface properties of carbon.