An effective method for synthesizing ZnS-core/carbon-sheath nanocables and nanocable-aligned ZnS tetrapod nanocrystals has been developed. Nanocable heterostructures and nanocable-linked ZnS tetrapods were synthesized in a controllable way. The tetrapods are single crystalline cubic ZnS with triangular-prism branches stretching out in four {111} directions. The tetrapods were aligned together with ZnS-C nanocables along the [100] direction.