The variegated aqueous chemistries of metal cations are applied to the design and synthesis of non-toxic solution precursors suitable for additive printing of large-area oxide electronics. Polycondensation behaviors of aqueous Al+3 and PO4+3 are manipulated in the deposition of atomically smooth amorphous aluminum oxide phosphate (AlPO) dielectric films. AlPO gate dielectrics with performance parameters not previously demonstrated via solution are integrated in thin-film transistors (TFTs). Simple zinc-ammine coordination chemistries enable low-temperature ink-jet printing of ZnO semiconductor films. Solution deposited ZnO films processed at low temperatures are integrated with AlPO dielectrics in high-performance TFTs. Discrete group 13 heterometallic hydroxo clusters are developed as aqueous precursors for InGaO3 semiconductor films. Insights from these polynuclear clusters are utilized in the synthesis of aqueous precursors for amorphous InGaZnO4 semiconductor films. These channels are similarly integrated with solution processed AlPO dielectrics on glass substrates, thereby demonstrating the potential for solution processed oxide macroelectronics.