Magnetic properties of Li
1−xNi
1+xO
2(0
x 0.08) crystallizing in the α-NaFeO
2structure were studied by SQUID magnetometry. A sample with
x 0.01 prepared from Li
2O
2and Ni
0.77O at 650°C follows the Curie–Weiss law from 350 to 80 K with μ
eff(effective Bohr magneton) of 1.91 μ
Band Θ (Weiss temperature) of +29.5 K. A spin glass-like thermomagnetic hysteresis with a cusp at 8 K was observed. Samples with larger
xvalues exhibit ferromagnetic moments, typically 0.3 μ
B/Ni (
x 0.08) at 5 K. From these and other results we conclude that the dominant intra-Ni layer interaction is ferromagnetic and that excess Ni ions located in the Li layers introduce strong ferromagnetic inter-Ni layer interactions. Possible importance of orbital–spin coupling and frustration in orbital ordering will be raised to the magnetism of ideal LiNiO
2, in which Ni
3+(
S