Gahnite from LCT granitic pegmatites of the Comechingones (Blanca Dora, Juan Román, Magdalena, La Ona, and Sin Nombre pegmatites) and Conlara (Nancy pegmatite) pegmatite districts, Argentina, was analyzed to investigate the relationship between its chemistry, pegmatite mineralogy, and pegmatite melt evolution. Based on the molecular proportions of endmembers (gahnite, hercynite, spinel, and galaxite) the composition of gahnite in these pegmatites is defined by the ranges Ghn77.7–91.0Hc7.4–20.0Spl0.25–3.37Glx0.7–2.4, which fall within the previously defined field for granitic pegmatites. Gahnite from the Nancy pegmatite has higher Mg and Mn contents than gahnite from the pegmatites of the Comechingones pegmatite district. Chemical variation within gahnite crystals is characterized by higher Zn (∼2.8 wt.% ZnO) and lower Fe (∼2.6 wt.% FeO) contents near the edge compared to inner portions, reflecting the evolution of the pegmatite melt via simple fractional crystallization. Other crystals show a complex zoning pattern of oscillations in Fe and Zn contents within the crystal and higher Zn and lower Fe near the rim compared to the core. A plot of molecular Fe2+ + Mg versus Zn + Mn yields a strong negative correlation and best displays the substitutions within the gahnite crystal structure and is the best to determine relative pegmatite melt evolution. Without implying a co-magmatic origin of the pegmatites, based on pegmatite mineralogy, Zn contents, Zn/Fe2+ ratios, and coupled Fe2++Mg and Zn+Mn values in gahnite, the relative degree of evolution of the pegmatites increases in the order: Sin Nombre → Magdalena → Juan Román → Blanca Dora → Nancy → La Ona. Based on the composition of gahnite in worldwide granitic pegmatites reported in the literature and those obtained here, the composition of gahnite in these rocks is defined by the endmember ranges Ghn50–98Hc1–50Spl0–7. This study shows that the major element composition of gahnite in granitic pegmatites can effectively be used to determine the relative degree of evolution of pegmatite-forming melts.