Core-shell type waterborne polyacrylate-polyurethane microspheres in which polyurethane acts as the shell and acrylic polymer as the core were prepared. Hydroxyethyl acrylate and adipic dihydrazide were used as cross-linking agents introduced to the ends of the shell molecular chains, and two kinds of cross-linked structures between the core and the shell were formed. The photon correlation spectroscopy studies indicate that all the microspheres present continuous particle-size distributions and their mean particle sizes are smaller than 200 nm. The transmission electron photographs reveal that there are obvious core-shell structures for the noncross-linked type microsphere particles and different cross-linked networks between the core and shell for the two kinds of cross-linked type microsphere particles. These microspheres possess excellent storage stability, water resistance, and coating properties.