An Ultra‐Robust and Crystalline Redeemable Hydrogen‐Bonded Organic Framework for Synergistic Chemo‐Photodynamic Therapy

and excellent chemical stability (intact in concentrated HCl for at least 117 days). A new method of acid-assisted crystalline redemption is used to readily cure the thermal damage to PFC-1. With periodic integration of photoactive pyrene in the robust framework, PFC-1 can efficiently encapsulate Doxorubicin (Doxo) for synergistic chemo-photodynamic therapy, showing comparable therapeutic efficacy with the commercial Doxo yet considerably lower cytotoxicity. This work demonstrates the notorious stability issue of HOFs can be properly addressed through rational design, paving a way to develop robust HOFs and offering promising application perspectives.