We report on ferroelectric/giant magnetoresistive Na0.5K0.5NbO3/La0.6Sr0.2Mn1.2O3 (NKN/LSMO) heterostructures grown onto LaAlO3 (001) single crystal using KrF pulsed laser ablation of stoichiometric ceramic target. Main processing parameters have been optimized to obtain smooth LSMO template layer, avoid NKN-LSMO interdiffusion, preserve NKN stoichiometry against the lost of volatile potassium and sodium and achieve reasonable reliability of NKN film performance. X-ray diffraction θ- 2θ scans and rocking curves evidence for single-phase content and high c-axis orientation both in template LSMO and top NKN layers. Ferroelectric measurements yield remnant polarization Pr
of 1.5 [C/cm2 and spontaneous polarization Ps
of 7 μC/cm2 at electric field strength of 130 kV/cm. At room temperature, dielectric permittivity ε′ and dissipation factor tan δ have been found to vary from 595 to 555 and 0.046 to 0.029 respectively in the frequency range of 0.4 to 20 kHz. At 10 kHz dielectric permittivity linearly increases from 410 to 650 in the temperature range 77 K to 415 K while the dissipation factor below 320 K does not exceed 3%.