The hydrolysis reaction between Brønsted basic organometallic or metal-amide reagents with Brønsted acidic OH groups from water or metal-hydroxides may act as a controlled stoichiometric strategy for the formation of M-O-M bonds, if careful consideration of reaction conditions is employed. This article explores the utilisation of highly reactive organometallic and metal-amide complexes from across the periodic table as reagents for the synthesis of metal-oxo clusters, oxo-bridged heterobimetallics and metal oxide nanoparticles. Such reactivity typically occurs at low temperatures with the release of hydrocarbon or amine by-products. The impact of ligand coordination, M-C bond strength, M-OH acidity and reaction temperature are discussed.