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Structure and dielectric/piezoelectric properties of the sol–gel-derived 0.36BiScO3–0.64PbTiO3 (BSPT) thin films deposited on Pt(111)/Ti/SiO2/Si(100) substrates with PbO seeding layers are investigated. Highly (100)-oriented BSPT thin films with thickness ranging from 250 to 950 nm were synthesized by alternatively coating PbO seeding layers and BSPT layers. The as-deposited BSPT film with thickness of 950 nm showed high dielectric constant of 1850 and effective piezoelectric coefficient d33* of approximate 150 pm/V, the latter was comparable with that of the (001) epitaxial BSPT films grown on Nb–SrTiO3 single crystal substrates. The influence of PbO seeds on the structure and electric properties of the films is discussed as well.