Due to their unique morphologies and surface properties, the raspberry-like core-shell composite particles, consisted of a central sphere surrounded by smaller spherical particles, have received significant attention and found various technological applications. The heterocoagulation of large and small particles is one of the most simple and widely used routes for the synthesis of raspberry-like composites in large scale because of its simplicity, versatility, and controllability. However, the weak interactions between the associated particles always result in the irreversible loss of the surface structures and functionalities in routine use.