Effective wastewater treatment remains a critical challenge, especially when dealing with hazardous pollutants like antimony (Sb(III)). This study addresses this issue by using innovative nanocomposites to remove Sb(III) ions from water, while simultaneously repurposing the spent adsorbents for energy storage applications. We developed reduced graphene oxide-NiFe2O3-SiO2-polyindole nanocomposites (RGO-NiFe2O3-SiO2-PIn NCs) via a hydrothermal synthesis method, achieving a high removal efficiency of 91.84% for Sb(III) ions at an initial concentration of 50 mg/L at pH 8. After adsorption, the exhausted adsorbent was repurposed for energy storage, effectively minimizing secondary pollution. The Sb(III)-loaded adsorbent (RGO-NiFe2O3-SiO2-PIn@SbOx) exhibited excellent performance as an energy storage material, with a specific capacitance (Cs) of 701.36 F/g at a current density of 2 A/g and a retention rate of 80.15% after 10,000 cycles. This dual-purpose approach not only advances wastewater treatment technologies but also contributes to sustainable and economical recycling practices, particularly in the field of energy storage.