Although sulfide‐based materials are known to be efficient catalysts for oxygen evolution reactions (OER), hydrogen evolution reactions (HER), and supercapacitor applications, improving the catalytic activity of sulfide materials for both electrochemical water splitting and supercapacitors remains a challenging problem. Here, an easy and one‐step integrated methodology is implemented to develop NiS/MoS2 anchored multiwall carbon nanotubes (MWCNT/NiS/MoS2) catalysts that can effectively and robustly catalyze both the HER and OER. The MWCNT/NiS/MoS2 hybrid composite offers the lowest overpotential of 201 mV and 193 mV to achieve a current density of 10 mA/cm2 and −10 mA/cm2 with a small Tafel slope of 58 mV/dec 41 mV/dec for OER and HER, respectively, in alkaline and acidic conditions. The obtained multi‐walled carbon nanotubes anchored with intertwined NiS/MoS2 have a significant number of active sites and defects throughout the structure. The hybrid composite electrode delivered a specific capacitance of >371.45 F/g at 2 A/g in a two‐electrode system, along with high energy density of 51.63 Wh/kg (ED) along with the power density (PD) of 953.63 W/kg, and good capacitance retention ∼82% after 2000 cycles. Therefore, a tandem electron transfer mechanism between NiS and MoS2 (MoS2→NiS) is believed to have an electrical synergistic effect that promotes both HER and OER activity. This research opens a new path for the construction of multi‐component, cheap electrocatalysts that are highly effective for overall water splitting and energy storage applications.