In this work, sulfur doped nickel cobalt layered double hydroxide nanosheet arrays are fabricated on a stainless steel (S-LDH/SS) substrate by simple electrodeposition technique for electrocatalytic hydrogen evolution reaction (HER) and supercapacitor applications. The surface morphology and chemical composition of S-LDH/SS are accessed by field emission electron microscopy (FE-SEM) with energy dispersive X-ray spectroscopy (EDX) and X-ray photoelectron spectroscopy (XPS), respectively. Remarkably, the fabricated S-LDH/SS electrode requires low overpotential of −0.38V vs. RHE to accomplish a current density of −10mAcm−2 with a less Tafel slope of −69mVdec−1 for HER in aqueous KOH. Further, the tailored S-LDH/SS behaves like a battery-type electrode and delivers maximum specific capacity of 344Cg−1 (95.5mAhg−1) at scan rate of 5mVs−1, which possess excellent cyclic stability and capacity retention. The S-LDH/SS comprised by two types of active catalytic sites along with anions furnish an excellent conductivity, which improving the mass and ionic transportations. Hopefully, exceptional electrochemical interpretation substantiates that this S-LDH/SS electrode might be a favorable material for the energy conversion and storage applications.