alpha-Ni(OH)(2) and Ni-Al layer double hydroxides (LDHs) precipitated by urea were investigated with FTIR and XPS. Possible modes of cyanate (CNO-) coordination during the nucleation and growth of precipitates is discussed. In the early stages, cyanate ion in R-Ni(OH)(2) is found mainly to be N-bonded to Ni2+ ions in the layers, whereas later in the growth stages, it is bonded through oxygen. In LDHs cyanate remains N-bonded. These changes in the coordinations modes are related to the decreasing supersaturation levels during digestion. XPS results support the FTIR results.