Synthesising and designing pseudocapacitive material with good electrochemical and electrocatalytic behaviour is essential to use as supercapacitor as well as non‐enzymatic glucose sensor electrode. In this work, NiCo2S4 nanoparticles decorated onto the 2D‐Carbyne nanosheets are achieved by the solvothermal process. The as‐prepared NiCo2S4@2D‐Carbyne provides rich reaction sites and better diffusion pathways. On usage as an electrode for supercapacitor application, the NiCo2S4@2D‐Carbyne exhibits the specific capacitance of about 2507 Fg‐1 at 1Ag‐1. In addition, the fabricated hybrid device generates an energy density of 52.2 Wh kg‐1 at a power density of 1.01 kW kg‐1. Besides, the glucose oxidation behaviour of NiCo2S4@2D‐Carbyne modified GCE has also been performed. The diffusion of glucose from the electrolyte to the electrode obeys the kinetic control process. Furthermore, the fabricated NiCo2S4@2D‐Carbyne non‐enzymatic glucose sensor exhibits a limit of detection of about 34.5 µM with a sensitivity of about 135 µA mM‐1cm‐2. These findings highlight the need to design and synthesis electrode materials with adequate electrolyte‐electrode contact, strong structural integrity, and rapid ion/electron transport.