Supercapacitors have aroused widespread interest as advanced electrochemical energy storage devices owing to their excellent electrochemical performances in terms of power density, rate capability, and cycling stability. In these devices, the electrode material is the most important component that determines the performance. Therefore, extensive efforts on robust and efficient electrode materials have been carried out. Metal sulfides and phosphides are emerging as potential candidates for advanced supercapacitors due to their superior electrical conductivity and higher theoretical capacitance than their oxide counterparts. However, severe volume expansion and sluggish reaction kinetics largely hinder their cycling stability and rate capability. To further improve their electrochemical performance, strategies including nanostructuring, compositing, and designing architecture of electrodes, etc. have been investigated. In this chapter, the synthesis methods of metal sulfides/phosphides are presented. Subsequently, advanced electrode materials based on metal sulfides/phosphides with various structures, morphologies, compositions, and electrochemical performances are highlighted and discussed. Finally, the conclusions, challenges, and prospects of metal sulfides/phosphides as efficient electrochemical energy storage materials are proposed.