Two novel chiral amino alcohol-nickel complexes (I) and (II) have been first reported from the direct reaction of L-plenylglycinol with Ni(OAc)2 · 4H2O in anhydrous ethanol and L-phenylalaninol with NiCl2 · 6H2O in anhydrous methanol. The crystal structures of I and II were determined by X-ray diffraction and further characterized by elemental analysis and IR. For I: C24H31N3NiO3, monoclinic, P21, a = 5.2581(12), b = 23.683(5), c = 13.744(3) Å, β = 97.939(6)°, V = 1695.1(7) Å3, Z = 2, ρcalcd = 0.917 g/cm3, the final R factor was R 1 = 0.0897, 5315 for reflections were observed with I 0 > 2σ(I 0); for II: C27H43Cl2N3NiO5, orthorhombic, P212121, a = 9.844(3), b = 12.373(3), c = 26.158(7) Å, V = 3186.3(14) Å3, Z = 4, ρcalcd = 1.291 g/cm3, the final R factor was R 1 = 0.0371, 6265 for reflections were observed with I > 2σ(I).