Heat capacities, magnetic susceptibilities, and X-ray diffraction patterns of Ni(OH)2 monolayer nanoclusters (Ni-MNC) in amorphous SiO2 synthesized with various concentration ratios of NiCl2 and Na2SiO3 solutions were measured. The Ni-MNCs exhibited a broad heat capacity anomaly around 20 K. Magnetic entropies for the Ni-MNCs were smaller than the expected value for S = 1 spin systems (Rln3 = 9.13 J K−1 mol−1), which suggests that the Ni-MNCs show a spin-glass-like behavior. Magnetic susceptibility measurements indicated change of the blocking temperature where the ZFC and FC data branched, which is characteristic of spin glass systems. X-ray diffraction experiments showed the direct evidence that the sizes of the Ni-MNCs are different by the synthetic condition.