Highly c-axis oriented single phase Na0.5K0.5NbO3(NKN) thin films have been deposited onto polycrystalline Pt80lr20substrates and SiO2/Si(001) wafers using pulsed laser ablation of stoichiometric ceramic target. Strong self-assembling of NKN films along the [001] direction has been observed. Properties of NKN/Pt thin film structures have been successfully tailored by oxygen pressure control from the ferroelectric state, characterized by the remnant polarization of 12 uC/cm2, dielectric constant ε ∼ 520 andtanδ ∼ 0.024 @ 100 kHz, to superparaelectric state withtanδ as low as 0.003 and ε = 210 with very small 1.7% dispersion in the frequency domain 0.4–100 kHz and less than 10% variation in the temperature range 77–415 K. NKN films grown onto SiO2/Si(001) substrates show quadrupled super-lattice structure alongc-axis, losstanδ less than 0.01, and ε ∼ 110 @ 1 MHz.C-V measurements for Au/NKN (270nm)/SiO2/Si MFIS-diode structure yield memory window of 3.26 V at the programmable voltage of 8 V.