The stacked single-unit cell Ba1-xSrxTiO3 (BSTO) thin film designed by the high-throughput method is fabricated by layer-by-layer deposition by laser molecular beam epitaxy, and its ferroelectric and dielectric characteristics as a function of Sr concentration are comprehensively investigated. The permittivity of BSTO exhibits a monotonous increase by Sr with a plateau in the region of 14% < Sr < 85%. Meanwhile, at the low Sr doping regime, the piezoelectric response has been discovered, and the maximum piezoresponse and d33 can reach approximately 139.05 pm and 88 pm/V once an appropriate Ba/Sr ratio is formed, exhibiting a coexistence of a dielectric property and giant piezoresponse. This effective piezoelectric constant d33 value is significantly larger than the conventional chemical doping scenarios, suggesting that the intra-plane interaction is crucial for designing future promising dielectric and ferroelectric thin films via high-throughput technologies.