Herein, we report three new composites containing multimetallic layered double hydroxides [Ni/Al LDH, Ni.Co/Al LDH, and Ni.Co/Al.Ce LDH] and bayerite/boehmite/ceria. In-situ composites formed in a one-pot solid-state reaction and characterization by powder XRD, FT-IR, FE-SEM, and EDS Spectroscopy. The powder XRD and FT-IR spectra indicate the presence of LDH, bayerite, boehmite, or ceria in the solid. The morphological characteristic of the composites demonstrated that the structure was layered material, and the EDS spectra confirmed that the multimetallic components were present in the composite.