Redispersible powders based on soft core-hard shell polymer particles can be used as additives in polymer-cement mortars. The role of this morphology on the spray-drying production of these powders and on the crack-bridging properties of the corresponding cement-based membranes is investigated. Different polymer latexes at high solid content with varied core-shell ratio, shell thickness and chemical composition (hardness) were prepared from styrene and 2-ethylhexyl acrylate monomers via semi-batch emulsion polymerization. The latexes were characterized in terms of size, composition, and glass transition temperature (T g ), and spray-dried to obtain redispersible polymer powders (RPPs) using poly (vinyl alcohol) and limestone powder as anti-caking agents. The polymer powders were mixed with a mortar mixture and redispersed in water to produce cement-based membranes, which were tested for crack-bridging properties at different temperatures. The results showed that it was not possible to spray-dry a dispersion of homogeneous polymer particles with T g of −25 ∘ C, unless these particles are protected by much harder (high T g ) shell. In particular, it was observed that a thicker shell improved the spray-ability, but lowered the crack-bridging properties of the produced membrane. A trade-off between these two was revealed to be the key for the optimal design of the polymer nanoparticles, as proven by the systematic study of the core-shell morphology reported in this work. The best compromise was shown to consist of particles larger than 300 nm, shell thickness of about 5 nm, and core-shell ratio of 97%, with styrene content in the shell not larger than 80% to avoid excessive hydrophobicity.