Metal-organic frameworks (MOFs) hold promise as efficient electrode materials for supercapacitors, but their practical application is hindered by the intrinsic low electrical conductivity. Here, we employ CO2-derived carbon nanotubes based on molten salt electrolysis (MSE-CNTs) as the framework to guide the growth of nickel-based MOF (Ni-MOF). The resulting MSE-CNTs/Ni-MOF composite exhibits an impressive specific capacitance of 1714.2 F g−1 at 1 A g−1, 1.45 and 1.26 times greater than bare Ni-MOF (1185.7 F g−1) and CVD-CNTs/Ni-MOF (1364.3 F g−1, the composite of Ni-MOF and commercial CNTs produced by chemical-vapor-deposition), respectively. Moreover, the assembled hybrid supercapacitor (MSE-CNTs/Ni-MOF//active carbon) achieves a remarkable specific capacitance of 136.5 F g−1 at 1 A g−1 and an energy density of 54.8 Wh kg−1 at 850 W kg−1, standing among the best of the state-of-the-art. The superior capacitive performance of MSE-CNTs/Ni-MOF than CVD-CNTs/Ni-MOF can be attributed to the better electrical conductivity of MSE-CNTs, the thinner nanosheet architecture of MSE-CNTs/Ni-MOF, and the effective electrically conductive network within the composite. This work marks a paradigm shift from greenhouse gas CO2 to excellent energy storage materials, paving the way for addressing both the energy and climate issues simultaneously.