Reported here are two new heterometallic chalcogenide supraclusters ([Ga56Sb16S136] and [In36Sb6S75]), which present new self-assembly modes of basic supertetraheral clusters with the assistance of antimony ions. This work demonstrates the crucial role of the added metal ions with nontetrahedral coordination geometry in developing supertetrahedral-cluster-based supraclusters with a new level of complexity.