​In this work, a pre-designed Zr-based-MOF encompassing an organic linker with a redox active core is synthesized and its structure–property relationship as a supercapacitor electrode is investigated. An enhanced performance is revealed by the combination of this MOF's high porosity and redox core incorporation, which alters its double-layer and pseudocapacitance, respectively. An increase in the capacitance performance by a factor of two is achieved via post-synthetic structure rigidification using organic pillars.