Two aluminate spinel materials (ZnAlO and NiAlO) were synthesized by the citrate precursor method. The citrate precursors consisting of coprecipitated citrates of Zn or Ni and aluminum were first subjected to thermal analysis (TG-DSC) for determining the optimum temperature for annealing. Two step decomposition was observed incorporating dehydration and formation of the aluminate. The second step gives an endo peak (−2937 J/g) at 356 °C in the DSC curve of the coprecipitated nickel(II) citrate-aluminum citrate gel in O atmosphere. Kinetic/mechanistic analysis of the TG data has also been carried out and values of E, Δ S, Δ G, and A were approximated. On the basis of the findings, 450 °C has been chosen for annealing of the gels. Annealing has also been done at 650 °C for 1 h in muffle furnace in an attempt to obtain nanometric particles of aluminates (MAlO) {M = Ni, Zn} and to find out their magnetic properties which could render them useful for chemical sensing applications, etc. The TG-DSC curves of various powders which were obtained on annealing at the two temperatures did exhibit thermal instability when carried out in N atmosphere. NiAlO and ZnAlO spinels (particle size 17 and 34 nm, respectively) are obtained in pure crystalline phase at 650 °C. ZnAlO prepared this way shows coercivity values of 470 and 58.37 G and NiAlO, 107 and 23.24 G when annealed at 450 and 650 °C, respectively. ZnAlO prepared by a polymer precursor method and annealed at 1000 °C, has earlier been reported to have coercivity value of 469 G. Thus, the citrate precursor method is good for the synthesis of ZnAlO, producing single phase nanocrystalline powder of high quality and crystallinity. The value of magnetization was found to be small in the present case for the NiAlO spinel obtained at 450 °C. [ABSTRACT FROM AUTHOR]