Muhammad Ahsan Farooq Qaisar, Salamat Ali, Salamat Ali, Inaam Ullah, Anand Parkash, Shaghfar Ali Malik, Ayesha Irfan, Shafqat Ali, Shafqat Ali, Jing Qi, Weihua Han
ABSTRACT Supercapacitors (SCs) are prized for their exceptional cycle life, operational stability, inherent safety, and maintainability. The electrolyte is a critical component, directly governing their electrochemical performance. This study investigates molybdenum disulfide (MoS 2 ) as a capacitive electrode material across chloride‐based electrolytes (LiCl, KCl, NaCl, ZnCl 2 ). Findings reveal that the divalent Zn 2+ ion enables significantly enhanced energy storage compared to monovalent cations. The MoS 2 electrode in the Zn 2+ ‐based electrolyte achieved a remarkably high specific capacitance of 630.5 F/g at 1 A/g, vastly outperforming LiCl, KCl, and NaCl (413.55, 281.94, and 275.73 F/g, respectively). It also demonstrated exceptional long‐term stability, retaining 97% of its initial capacitance after 10 000 charge–discharge cycles. Density functional theory (DFT) calculations corroborate these results, indicating a stronger adsorption interaction between Zn 2+ ions and the MoS 2 , which elucidates the superior charge storage. To demonstrate practical viability, an asymmetric SC (MoS 2 //CP) was assembled. This device delivered a high capacitance of 260.5 F/g at 1 A/g and maintained ∼ 93% of its capacity over 10 000 cycles within a 0.0–1.6 V voltage window. This work provides fundamental insights and a promising pathway for developing high‐performance, durable MoS 2 ‐based Zn 2+ ‐ion SCs, advancing the field of advanced energy storage solutions.