Ba0.6Sr0.4TiO3 (BST) and 0.06Nd(Zn1/2Ti1/2)O-3-0.94Ba (x) Sr1-x TiO3 (NZT-BST) thin films with x = 0.6, 0.7, 0.75, and 0.8 were fabricated on Pt/Ti/SiO2/Si substrates by sol-gel method. The structures, surface morphology, dielectric, and ferroelectric properties, and thermal stability of BST and NZT-BST thin films were investigated as a function of NZT and Ba content. It was found that introducing NZT into BST decreased significantly dielectric loss, however, along with the tunability. On this basis, increasing Ba/Sr in NZT-BST thin films led to the simultaneous increase of dielectric constant and tunability of thin films. As a result, optimized dielectric and tunable properties were obtained for 0.06Nd(Zn1/2Ti1/2)O-3-0.94Ba(0.7)Sr(0.3)TiO(3) thin film with the highest FOM value of 43.22. It awakens us that, for reducing dielectric loss, introducing a certain amount of low permittivity oxides or non-ferroelectrics like NZT into weak ferroelectric perovskite tunable materials, not into paraelectric perovskite tunable materials, may obtain more excellent dielectric and tunable performances.