The synergistic effect between multi-component electrode materials often makes them have better lithium storage performance than single-component electrode materials. Therefore, to enhance surface reaction kinetics and encourage electron transfer, using multi-component anode materials is a useful tactic for achieving high lithium-ion battery performance. In this paper, ZnS/ZnO composites were synthesized by solvothermal sulfidation and calcination using metal-organic frameworks as sacrificial templates. From the point of materials design, both the ZnS and ZnO have high theoretical specific capacities, and the synergistic effect of ZnS and ZnO can promote charge transport. From the perspective of electrode engineering, the loose porous carbon skeleton formed after calcination of metal-organic frameworks can not only improve the conductivity of composite materials, but also facilitate the full penetration of electrolyte, expand the contact area between electrolyte and active material, which are all conducive to improving the lithium storage performance. As expected, ZnS/ZnO anode materials showed ultra-high specific capacity and excellent rate performances. Combining material design and electrode engineering, the paper provides another idea for preparing high performance anode materials for lithium-ion batteries.