Two‐dimensional (2D) metal–organic frameworks (MOFs) have been a worldwide research interest due to their potential application in supercapacitors. Herein, a cobalt‐based layered MOF ([Co2(μ‐SO4)(Hppza)2(H2O)3]n, namely, SEU‐1; H2ppza = 3‐(pyridin‐4‐yl)‐1H‐pyrazole‐5‐carboxylic acid) has been synthesized via a one‐step solvothermal method. Single X‐ray diffraction analysis shows that the SEU‐1 exhibits a (3,3,4)‐connected 2D structure with a Schläfli symbol of (62·8)(63)(64·8·10). Variable‐temperature magnetic susceptibility data display that antiferromagnetic interactions between two CoII ions exist in SEU‐1. The supercapacitive performance has been evaluated in the three‐electrode system. Its maximum specific capacitance is 145.5 F g−1 at 1 A g−1, along with the specific capacitance retention of 92.7% at the current density of 5 A g−1 after 6000 cycles in 3 M KOH solution. These results demonstrate that SEU‐1 is a good candidate for electrode material for electrochemical energy storage.