Some recent reports claiming room temperature spontaneous magnetization in layered double hydroxides (LDHs) have been published; however, the reported materials cause serious concern as to whether this cooperative magnetic behavior comes from extrinsic sources, such as spinel iron oxide nanoparticles. The syntheses of crystalline Fe3+-based LDHs with and without impurities have been developed, highlighting the care that must be taken during the synthetic process in order to avoid misidentification of magnetic LDHs.