Nanozyme-based tumour catalytic therapy has attracted widespread attention in recent years, but the therapeutic efficacy is limited due to the trapping of hydroxyl radicals (˙OH) by endogenous glutathione (GSH) in the tumour microenvironment (TME). Zr/Ce-MOFs/DOX/MnO2 is constructed in this work to serve as a new kind of nanozyme for combination chemotherapy and catalytic treatment. Zr/Ce-MOFs can produce ˙OH in a mimic TME, and the MnO2 on the surface could deplete the GSH, further promoting the ˙OH generation. The pH/GSH dual stimulation accelerates the release of anticancer drug doxorubicin (DOX) in tumour tissue for enhanced tumour chemotherapy. Moreover, Mn2+ produced by the reaction of Zr/Ce-MOFs/DOX/MnO2 and GSH can be used as the contrast agent for T1-MRI. The potential antitumour effect of Zr/Ce-MOFs/DOX/MnO2 is demonstrated by in vitro and in vivo cancer treatment tests. This work thus provides a new nanozyme-based platform for enhanced combination chemotherapy and catalytic treatment for tumours.