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Lead-free potassium sodium niobate (K0.5Na0.5)NbO3 thin films on Pt(111)/TiO2/SiO2/Si substrates have been prepared from the acetate–alkoxide-based precursor solutions with the stoichiometric composition and with 5 or 10 mol% excess of sodium or potassium acetate. Upon heating to 750°C, the films crystallize in pure perovskite phase. The increasing amount of alkali excess in solutions increases the degree of {100} orientation and it influences the nucleation and growth processes in the films. The microstructure of about 250 nm thick films prepared from the stoichiometric and 5 mol% excess solutions consists of equiaxed grains of about 50 nm across, whereas the grain size in the about 220 nm thick films prepared from the 10 mol% excess solutions is about 200 nm. The energy dispersive X-ray spectroscopy revealed that the alkali excess in precursor solutions contributed to a higher level of chemical homogeneity of the films on the micrometer scale. The chemical composition of the films prepared from the 5% potassium-excess solution was closest to the (K0.5Na0.5)NbO3 composition among all the samples as a result of more pronounced potassium losses upon heating. These films had the room temperature values of dielectric permittivity, dielectric losses, remnant polarization, and coercive field measured at 1 kHz 610, 0.015, 8 μC/cm2, and 80 kV/cm, respectively.