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Lead-free sodium–potassium niobate-based piezoelectric materials are most intensively studied in order to replace the widely used Pb-based ones. In this work, the effects of modification of compositions by donor and acceptor dopants in the A- and B-sites of perovskite lattice on structure, dielectric, ferroelectric, and piezoelectric properties of ceramics from Morphotropic Phase Boundary in the (1−x)(K0.5Na0.5)NbO3–xBaTiO3 system and in compositions with x=0.05 and 0.06 additionally doped by Ni3+ cations have been studied.