Crystalline nanosheets were successfully formed on magnesium alloy AZ31 by a facile surfactant-free hydrothermal treatment using aqueous solution. The crystal structures and shapes of the nanosheets changed with the treatment temperature. On treatment at 120 °C, rosette-like structures made from curved nanosheets of crystalline Mg1−xAlx(OH)2(NO3)x·nH2O were formed. At 150 °C, plate-like nanosheets of crystalline Mg1−xAlx(OH)2(NO3)x·nH2O and Mg(OH)2 were formed. Further increase in the treatment temperature to 180 °C yielded larger crystals with sharp edges. The crystallites were crystalline Mg(OH)2 with a distinct plate-like shape with the edges preferentially directed out of the magnesium alloy. The formation mechanism of this morphology is also discussed.