Zinc sulfide (ZnS) is a promising anode material for lithium-ion batteries (LIBs) because of its high theoretical capacity, abundance, cost-effectiveness, and environmental friendliness. Herein, a hydrangea-like ZnS-carbon composite (ZnS-NC) is synthesized through the hydrothermal method and subsequent pyrolysis of a supramolecular precursor guanosine. The resulting composite comprises ultrafine ZnS nanoparticles firmly stabilized on a nitrogen-doped carbon matrix, featuring mesoporous channels and high surface areas. When utilized as an anode material for LIBs, the initial discharge specific capacity of the ZnS-NC electrode reaches an impressive value of 944 mA h g-1 at 1.0 A g-1, and even after 450 cycles, it maintains a reversible capacity of 597 mA h g-1. Compared with pure ZnS, the ZnS-NC composite exhibits significantly improved rate performance and cycling stability. This enhancement in Li-storage performance can be attributed to a synergistic effect within the ZnS-NC composite, which arises from the large exposed active site area, efficient ion/electron transfer, and strong interaction between the ZnS nanoparticles and the carbon framework. Overall, this work presents an eco-friendly approach for developing metal sulfide-carbon composites with exceptional potential for energy storage applications.