Lead-free ferroelectric ceramics have been studied intensively, as possible applications range from the substitution of lead-based materials in piezoelectric devices to innovative cooling technologies by the exploitation of caloric effects. However, their full potential has not yet been revealed, neither in bulk materials, nor in case of thin films. This work presents the processing and analysis of K0.5Na0.5NbO3 samples on the basis of bulk and thin film materials. Hereby the influence of fabrication parameters, change of composition and doping with lithium niobate and manganese on the bulk material is studied and evaluated towards application in thin films fabricated by pulsed laser deposition. The structural evaluation focusses the analysis of the phase transitions and their optimization by application of the cofactor conditions, which allow for the very precise determination of favourable lattice structures in terms of material property enhancement.