This study investigates how variations in substrate temperatures and deposition rates during pulsed laser deposition on Nb-doped SrTiO3 substrates affect the crystallinity, and consequently, the ferroelectric and piezoelectric properties of SrBi2Ta2O9 (SBT) thin films. The SBT thin film developed at 850 °C with a deposition rate of 0.34 nm/pulse showed lower remanent polarization and piezoelectric coefficients, a result of its c-oriented crystallinity. In contrast, SBT thin films produced at 750 °C with deposition rates of 0.37 nm/pulse demonstrated enhanced ferroelectric and piezoelectric responses due to mixed a-oriented crystallinity. In particular, the SBT thin film, fabricated at 750 °C with a lower deposition rate of 0.04 nm/pulse, demonstrated the most enhanced ferroelectric and piezoelectric properties due to its highly refined a-oriented crystallinity. Our findings illuminate the relationship between the characteristics of the crystals and functional properties in SBT thin films, highlighting the integration of a-domains within c-domains as a key strategy for optimizing SBT film performance and opening avenues for designing specialized Bi-layered perovskite thin films. Display omitted •Fabricated SBT thin films via PLD on Nb:STO substrates with varied conditions.•Crystal structure and surface morphology crucially affect ferroelectric and piezoelectric properties.•Optimal SBT film performance achieved through integration of a-domains within c-domains.