We reviewed trends in composition, structure, and optoelectronic properties of inorganic phosphosulfides, aided by the existing literature and the Materials Project database. Based on this analysis, we assessed their potential as semiconductors for optoelectronic energy conversion applications. We believe that phosphosulfides deserve much closer research attention, as this material family likely contains semiconductors with strong light absorption and favorable charge transport and recombination properties. The main arguments leading to this recommendation are the following: 1) Among the known phosphosulfides, the majority are semiconductors with band gaps in the visible and threedimensional structural networks, indicating their potential to absorb relevant fractions of the solar spectrum and to ensure good electronic transport in all directions. 2) Direct-gap, low-effective-mass semiconductors are already known in ternary phosphosulfide systems (e.g., Ag 3 PS 4 , Ba 4 P 2 S), even though 3D structural networks in PSs do not always translate to low effective masses.