Organic-inorganic nanocomposites composed of polymers and nanoparticles offer a vast design space of potential material properties, depending heavily on the properties of these two constituents and their spatial arrangement. The ability to place polymers in direct contact with functional nanoparticles via strong bonding, that is, stable chemical interaction without the dissociation of surface capping polymers, provides a means of preventing nanoparticles from aggregation and increasing their dispersibility in nanocomposites, and promises opportunities to explore new properties and construction of miniaturized devices. However, this is still a challenging issue and has not yet been largely explored. Here, we report an unconventional strategy to create in situ organic-inorganic nanocomposites comprising monodisperse ferroelectric nanoparticles directly and permanently tethered with ferroelectric polymers by capitalizing on rationally designed amphiphilic star-like diblock copolymer as nanoreactors. The diameter of ferroelectric nanoparticles and the chain length of ferroelectric polymers can be precisely tuned. The dielectric and ferroelectric properties of nanocomposites containing different sizes of ferroelectric nanoparticles were scrutinized. Such bottom-up crafting of intimate organic-inorganic nanocomposites offers new levels of tailorability to nanostructured materials and promises new opportunities for achieving exquisite control over the surface chemistry and properties of nanocomposites with engineered functionality for diverse applications in energy conversion and storage, catalysis, electronics, nanotechnology, and biotechnology.