Mesenchymal stem cell (MSC) membrane‐coated metal–organic frameworks (MOFs) represent an innovative approach to enhance the uptake and therapeutic efficacy of copper‐based MOFs (Cu‐MOFs) in tumor cells. By leveraging the natural homing abilities and biocompatibility of MSC membranes, Cu‐MOFs can be effectively targeted to tumor sites, promoting increased cellular uptake. This coating not only facilitates superior internalization by cancer cells but also augments the therapeutic outcomes due to the enhanced delivery of copper ions. In vitro studies demonstrate that MSC membrane‐coated Cu‐MOFs (MSC‐Cu‐MOFs) significantly improve the cytotoxic effects on tumor cells compared to uncoated Cu‐MOFs. This novel strategy presents a promising avenue for advancing the precision and effectiveness of cancer treatment modalities, showcasing potential for clinical applications in oncology.