Supercapacitors have emerged as a promising class of energy storage technologies, renowned for their impressive specific capacities and reliable cycling performance. These attributes are increasingly significant amid the growing environmental challenges stemming from rapid global economic growth and increased fossil fuel consumption. The electrochemical performance of supercapacitors largely depends on the properties of the electrode materials used. Among these, iron-based sulfide (IBS) materials have attracted significant attention for use as anode materials owing to their high specific capacity, eco-friendliness, and cost-effectiveness. Despite these advantages, IBS electrode materials often face challenges such as poor electrical conductivity, compromised chemical stability, and large volume changes during charge–discharge cycles. This review article comprehensively examines recent research efforts aiming at improving the performance of IBS materials, focusing on three main approaches: nanostructure design (including 0D nanoparticles, 1D nanowires, 2D nanosheets, and 3D structures), composite development (including carbonaceous materials, metal compounds, and polymers), and material defect engineering (through doping and vacancy introduction). The article sheds light on novel concepts and methodologies designed to address the inherent limitations of IBS electrode materials in supercapacitors. These conceptual frameworks and strategic interventions are expected to be applied to other nanomaterials, driving advancements in electrochemical energy conversion.