This study aims at the deposition of PbTiO3 (PT) islands prepared by a water-based chemical solution deposition (CSD). Two aqueous citrato-based PbTiO3 precursor solutions, either with or without peroxide, are deposited by spin coating. The effect of different substrates on the formation of separated grains or islands is examined. It is observed that spin coating of a 0.6 M precursor solution on a Pt(1 1 1)/IrO2/Ir/SiO2/Si substrate gives the best results towards island formation. For this substrate, crystallizations are carried out between 600 °C and 900 °C. A final crystallization at 800 °C results in the highest degree of separation for the islands, while keeping the platinized substrate intact. The deposition of diluted precursors shows that it is possible to form islands from a precursor solution with a concentration down to 0.3 M. Solutions with a lower concentration result in irregularly shaped structures.