The heterolayered BT/BNT thick films were fabricated by screen printing techniques on alumina substrates electrodes with Pt. We report the improved ferroelectric and dielectric properties in the heterolayered tetragonal/rhombohedral structure composed of the BT and the BNT thick films. We investigated the effects of deposition conditions on the structural and electrical properties of the heterolayered BT/BNT thick films. The dielectric properties of the heterolayered BT/BNT thick films were superior to those of single composition BNT, and those values for the heterolayered BT/BNT thick films were 1455, 0.025 and $12.63 {mu}C/cm^2$.