GPC1 mAb clone 01a033 was labeled with Zr or At with a deferoxamine or decaborane linker, respectively...Internalization inhibitors (prochlorperazine) significantly inhibited the therapeutic effect of [At]GPC1 mAb, suggesting an essential role in targeted α-therapy. [Zr]GPC1 mAb PET showed high tumoral uptake in the early phase after administration, and targeted α-therapy using [At]GPC1 mAb showed tumor growth suppression. GPC1 is a promising target for future applications for the precise diagnosis of pancreatic ductal adenocarcinoma and GPC1-targeted theranostics.