NiAl layered double hydroxides (LDHs) are promising bifunctional catalysts comprising tunable redox and Lewis acidic sites. However, most studies of LDH employ alkali hydroxide carbonate precipitants which may contaminate the final catalyst leach into reaction media. Here, we report an alkali-free route to prepare NixAl LDHs with a composition range x = 1.7 4.1 using (NH4)2CO3 NH4OH as precipit...