Structure and dielectric/piezoelectric properties of the sol-gel-derived 0.36BiScO(3)-0.64PbTiO(3) (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 d(33)* 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.