Golf balls of the invention include at least one core layer comprised or consisting of a homogenous rubber-based core composition with a plurality of functionalized inorganic aluminosilicate ceramic microspheres dispersed throughout without agglomerating to create a relatively higher cross-link density of the core layer material. In golf balls of the invention, cross-link density gradients may be created between core layers by pre-electing the presence/absence, amount, type, and degree of functionalization of the plurality of functionalized inorganic aluminosilicate ceramic microspheres in two given core layers to target important properties such as resilience/CoR and desired playing characteristics such as distance.