Lead-free piezoelectric materials have grown in importance through increased environmental concern and subsequent EU and worldwide legislation, with the aspiration to reduce the use of Pb-based materials in all sectors. Integration of the next generation of lead-free piezoelectric materials with substrates to form functional micro devices has received less attention. Low temperature synthesis methods for K0.5Na0.5NbO3 (KNN) powder were developed to overcome the issue of poor purity of the final product during high temperature sintering. Molten hydroxide synthesis (MHS), derived from molten salt synthesis (MSS), has been developed to overcome a Na ion preference in the molten salt synthesis reaction that leads to NaNbO3 production instead of KNN when stoichiometric amounts of precursors are used. MHS makes use of a KOH molten reaction aid in place of the NaCl/KCl molten salt mix of the MSS. In a two stage reaction K rich intermediate niobates are produced and subsequent reactions with Na species produce KNN.