The poly(methyl methacrylate)-block-poly(methacrylic acid) diblock copolymer with different monomer compositions was synthesized via reversible addition fragmentation chain transfer polymerization. Meanwhile, a novel self-embrittling strippable coating was prepared using the diblock copolymers, which is proposed to be used as radioactive decontamination agents without manual operation. Furthermore, the decontamination efficiencies of self-embrittling strippable coatings for radioactive contamination on glass, marble, and stainless steel surfaces were studied.