Polymerisation-induced self-assembly (PISA) provides an efficient strategy that allows in situ polymerisation and simultaneous self-assembly of amphiphilic block copolymers at high solid contents. This thesis investigates several new aspects of PISA and extends the scope of preparation of nano-objects. We use ultrasound as a new initiation method for PISA to prepare nano-objects, as well as hybrid nanoparticles with catalytic properties; meanwhile, we synthesise rarely achieved “colloidal molecules” using thermal-PISA and hierarchical self-assembly.