In this study, the MET@CaP‐GOx‐PEG‐cRGD was observed to effectively inhibit the growth of two αvβ3 integrin over‐expressed tumor cell lines (HepG2 and B16F10 melanoma cells) via regulating the PP2A‐GSK3β‐MCL‐1 axis, and good cytocompatibility to the normal LO2 cells that low expressed αvβ3 integrin and GSK3β. Here, PTPA is linked to neoplasm.