Lithium-iron methasilicate (LiFeSi2O6, LFS), a member of clinopyroxene family, is an attractive compound for its multiferroic properties and applicability in energy-related devices. Conventional preparative method requires heating at elevated temperatures for long periods of time, with inevitable severe grain growth. We demonstrate that a-FeO(OH) (goethite) is superior as an iron source toward phase pure LFS over conventional hematite, a-Fe2O3. The exact phase purity, i.e., no trace of iron containing reactant, is confirmed in the goethite-derived LFS by 57Fe Mössbauer spectroscopy. The grain growth of LFS during heating is suppressed to keep its crystallite size of 120 nm. Higher reactivity of goethite in comparison with hematite is mainly attributed to the dehydration of goethite, which in our case was accelerated by Li2O. Related reaction mechanisms with the possible product pre-nucleation during mechanical activation are also mentioned. The magnetic properties of goethite-derived LFS are equivalent to those prepared via a laborious solid-state route. Thus, the presented preparative method offers a more sustainable route than conventional processing, and thus enables practical application of LFS. © 2020 Elsevier Ltd and Techna Group S.r.l.