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As a class of solid solution material, K(Ta,Nb)O3(KTN) single crystals have attracted significant interest due to their excellent piezoelectric and electro-optic performance. In this study, the piezoelectric properties of KTN were improved through Cu doping. Utilizing the advantages of composition-regulating phase transition, a large, high-quality Cu:KTN crystal measuring 30 mm × 25 mm × 20 mm in size was grown using the improved top seeded solution growth method. Cu-doped KTN exhibited better piezoelectric properties than pure KTN, and the full matrix parameters were investigated. Excellent dielectric, piezoelectric, and electromechanical coupling responses (ε11T∼2,136, d33∼303 pC/N, kt∼0.515, and k33∼0.672) were successfully obtained. To realize the optimized orientation of the piezoelectric properties, the orientation dependence of the single domain properties was investigated, and the mechanism of Cu doping to improve piezoelectric properties was explored. We found that 0.36% (in mass) Cu doped crystal consisted of A-site substitution, following ferroelectric and domain analysis. The small ferroelectric domain sizes led to a large domain wall mobility rate and high domain wall density, which contributed to high piezoelectric properties. This work revealed the effect of A-position doping on piezoelectric properties and provided a theoretical and experimental foundation for the performance optimization of KTN-based materials.