The properties of metal organic frameworks (MOFs), surface area, porosity, and functionality make them an ideal material for heterogenous catalysis. We developed a MnO2@quasi-MOF (MnO2@q-MOF) catalyst by incorporating MnO2 into a MIL-53 (Fe) structure with reduction of KMnO4 to MnO2 followed by a mild heat treatment at 300 °C. MnO2@q-MOF showed higher exposed metal sites due to thermally induced decarboxylation and higher activity because of in situ MnO2 formation while preserving the porosity and crystalline structure of MIL-53 (Fe). We activated potassium peroxymonosulfate (PMS) using our MnO2@q-MOF catalyst for decomposition of methylene blue and HEPES in water. The MnO2@q-MOF catalyst outperformed both MIL-53 (Fe) and unsupported MnO2 in the degradation of dye and was reusable. The primary mechanism of PMS activation was revealed to be a singlet oxygen (1O2) mediated process.