Curable silsesquioxane polymers are described comprising a core comprising a first silsesquioxane polymer and an outer layer comprising a second silsesquioxane polymer bonded to the core. The silsesquioxane polymer of the core, outer layer, or combination thereof comprises ethylenically unsaturated groups. The first silsesquioxane polymer of the core is bonded to the second silsesquioxane polymer of the outer layer via silicon atoms bonded to three oxygen atoms. In some embodiments, the outer layer has a higher concentration of ethylenically unsaturated groups than the core. In this embodiment, the core may be substantially free of ethylenically unsaturated groups. In other embodiments, the core has a higher concentration of ethylenically unsaturated groups than the core. In this embodiment, the outer layer may be substantially free of ethylenically unsaturated groups. The core and outer layer each comprise a three-dimensional branched network of a different silsesquioxane polymer. The silsesquioxane polymers of the core and outer layer may be homopolymers or copolymers. Also described are methods of preparing curable silsesquioxane polymer comprising a core and outer layer bonded to the core, articles comprising curable or cured compositions comprising the silsesquioxane core/outer layer polymers, and methods of curing.