An intrinsic room‐temperature coercivity of 7.45 kOe has been found in melt‐spun Nd0.4Fe0.6; this value is the largest ever reported for a rare‐earth–iron alloy. A significant correlation was found between quench rate and coercivitiy, suggesting that the quenched alloys consist of fine crystallites or clusters, whose average particle size can be matched to the single‐domain optimum by the appropriate quench rate.