Tunable ferroelectric capacitors, which exhibit a decrease of the dielectric permittivity (ϵ) under electric field, are widely used in electronics for RF tunable applications (e.g., antenna impedance matching). Current devices use barium strontium titanate as the tunable dielectric, and the need for performance enhancement of the tunable element is the key for device improvement. We report here on libraries of Ba0.97Ca0.03Ti1−xZrxO3thin films (0 ≤ x ≤ 27%) with a thickness of about 130 nm deposited on IrO2/SiO2/Si substrates using combinatorial pulsed laser deposition allowing for gradients of composition on one sample. A total of 600 capacitors on a single sample were characterized in order to statistically investigate the dielectric properties. We show that the tunabilty is maximum at intermediate compositions, reaching values up to 60% for an electric field of about 400 kV cm−1. We attribute the high tunability in the intermediate compositions to the paraelectric-ferroelectric phase transition, which is brought down to room temperature by the addition of Zr. In addition, the piezoelectric coefficient is found to be decreasing with increasing Zr content.