One-dimensional (1D) hybrid nanostructures composed of silver/silver sulfide (Ag/Ag2S) and zinc sulfide (ZnS) were prepared by controllable migration of Ag species from the Ag nanowire (NW) core into the ZnS nanosheet shell. This Ag diffusion process can be manipulated by different concentrations of sulfur (thiourea) to realize various interspersion of Ag2S with ZnS. Because of the homogeneous dispersion of Ag with ZnS at the lattice scale, the as-formed 1D nanostructures have demonstrated red/blue light- enhanced electrocatalytic properties for water splitting. In addition, the Ag interspersion has enabled ZnS sensitivity to visible light, which results in efficient 1D hybrid materials for photocatalytic hydrogen (H-2) production under visible light. In this work, we have designed and explored an Ag migration method to prepare 1D core-shell nanostructures for bifunctional catalysis.