Metal–organic frameworks (MOFs) with redox metal centers have come into view as potential materials for electrochemical energy storage. However, the poor electrical conductivity largely impedes the potentiality of MOFs to construct high-performance electrodes in supercapacitors. In this work, a self-dissociation strategy has been applied to construct Ni-MOF microbelts on Ni foam (NF), where the NF is used as both a support and a Ni source. The transmission channels between the Ni-MOF and NF are favorable for the charge transport due to the in situ self-assembly of the TPA linkers with the dissociated Ni ions from the Ni foam. The grown Ni-MOF microbelt arrays can offer abundant active sites for redox reactions. The prepared Ni-MOF/NF-s electrode can yield a high capacitance of 1124 F g−1 at 1 A g−1 and retains 590 F g−1 at 10 A g−1. This design may offer a controllable protocol for the construction of MOF microbelt arrays on various metal substrates.