An atomic-layer-deposited Al2O3/HfO2/Al2O3 (A/H/A) tunnel barrier is investigated for Co nanocrystal memory capacitors. Compared to a single Al2O3 tunnel barrier, the A/H/A barrier can significantly increase the hysteresis window, i.e., an increase by 9 V for ±12 V sweep range. This is attributed to a marked decrease in the energy barriers of charge injections for the A/H/A tunnel barrier. Further, the Co-nanocrystal memory capacitor with the A/H/A tunnel barrier exhibits a memory window as large as 4.1 V for 100 μs program/erase at a low voltage of ±7 V, which is due to fast charge injection rates, i.e., about 2.4 × 1016 cm−2s−1 for electrons and 1.9 × 1016 cm−2s−1 for holes.