Nanodielectrics is an emerging field with applications in capacitors, gate dielectrics, energy storage, alternatives to Li-ion batteries, and frequency modulation in communications devices. Self-assembly of high k dielectric nanoparticles is a highly attractive means to produce nanostructured films with improved performance—namely dielectric tunability, low leakage, and low loss—as a function of size, composition, and structure. One of the major challenges is conversion of the nanoparticle building block into a reliable thin film device at conditions consistent with integrated device manufacturing or plastic electronics. Here, the development of BaTiO3 and (Ba,Sr)TiO3 superparaelectric uniform nanocrystal (8–12 nm) films prepared at room temperature by evaporative driven assembly with no annealing step is reported. Thin film inorganic and polymer composite capacitors show dielectric constants in the tunable range of 10–30, dependent on composition, and are confirmed to be superparaelectric. Organic thin film transistor (TFT) devices on flexible substrates demonstrate the readiness of nanoparticle-assembled films as gate dielectrics in device fabrication.