The extraordinarily high capacity exhibited by lithium-rich oxides has motivated intensive investigations towards both the cationic and anionic redox processes. With recent main focus on the anionic redox behavior, the anionic redox chemistry has emerged as a new orientation to pursue higher-energy cathodes for lithium-ion batteries. However, the key practical issues such as voltage decay, voltage hysteresis, and irreversible oxygen loss of lithium-rich oxides have triggered researchers to act on the ligand by designing novel lithium-rich sulfides/selenides. In light of this, we herein provide a timely and in-depth perspective on the development of these lithium-rich sulfides/selenides with various structures and coordinations. We highlighted both the variations of phases and structures, lithium storage mechanism, detailed change of sulfur/selenide through anionic redox, and potentials for higher energy densities. We also outlined the main academic and commercial obstacles or challenges for these Li-rich sulfides/selenides for next-generation lithium-ion batteries.