The ferroelectric and piezoelectric properties of doped potassium tantalum niobate crystals with different Fe doping amounts and the adjustability of the properties are investigated. The hysteresis loops and current density curves show that the defect dipoles have an obvious effect on domain reorientation, and the effect decreases with increasing doping amount. The ferroelectric and piezoelectric properties can be adjusted via the defect dipoles, and the adjustability is reduced with increasing doping amount. A change of the doping amount leads to defect dipole structure evolution in the crystals, in which the defect dipoles transform from a polar structure to a nonpolar structure, which is the reason for the transition of the domain reorientation determined by the defect dipoles. This result has proved that introducing defects is an effective way to improve and regulate perovskite properties, and the doping amount is one of the important factors controlling the defect dipoles.