Controlling the position of metal sulfide architectures is prerequisite and facilitates their device applications in solar cells, light-emitting diodes, and many other optoelectronic fields. Thanks to ambient-connected gas network trapped upon superhydrophobic surfaces, H2S gas can be continuously transported and reacted with metal ions along solid/liquid/gas triphase contact interface. Therefore, precisely positioning metal sulfide microstructure arrays are generated accordingly. The growth mechanisms as well as influencing factors are investigated to tailor the morphology, structure, and chemical composition of these metal sulfide materials. This interface-mediated strategy can be widely applied to many other metal sulfides, such as PbS, MnS, Ag2S, and CuS. In particular, heterostructured metal sulfide architectures, such as PbS/CdS concentric microflower arrays, can be generated by stepwise replacement of metal ions inside liquid, exhibiting the advanced applications of this interface-mediated growth strategy.