Phosphorus (P) is a major impurity in goethite-rich iron ores and significantly reduces steel quality while increasing the energy and carbon costs of downstream processing. As global iron ore production increasingly relies on goethitic resources, there is growing interest in low-temperature, low-carbon approaches capable of selectively removing structurally bound P. Fe(II)-catalysed recrystallisation has recently emerged as a promising mechanism for mobilising impurities from Fe(III) oxides through coupled electron transfer, atom exchange, and mineral restructuring. This study investigates the effectiveness of Fe(II)-catalysed recrystallisation for dephosphorisation of two contrasting Pilbara goethitic ore microtypes: a relatively crystalline, Fe-rich goethite (GOL) and a structurally disordered, Al-Si-rich vitreous goethite containing significant amorphous material (GOV). Ore mineralogy and impurity speciation were characterised using X-ray diffraction (XRD), X-ray fluorescence (XRF), Mössbauer spectroscopy, Raman spectroscopy, synchrotron X-ray absorption spectroscopy (XAS), and aqueous geochemistry before and after reaction with aqueous Fe(II) under anoxic circumneutral conditions. Both ores exhibited rapid Fe(II) uptake and transient P mobilisation; however, the extent of P redistribution was strongly controlled by mineralogical architecture. The more crystalline GOL ore underwent greater Fe atom exchange and sustained recrystallisation, resulting in substantial transfer of P into alkali-extractable pools. Following 30 days of reaction, approximately 80 per cent of total P became extractable by 1 M NaOH, compared with ~25 per cent in untreated controls. In contrast, the more Al-Si-substituted and partially amorphous GOV ore exhibited rapid P re-sequestration and achieved only ~40 per cent extractable P. Aluminium remained largely immobile (