Mn-doped alumina red pigment was prepared with Mn(NO3)2·6H2O and Al(NO3)3·9H2O as main raw materials by Low-temperature Combustion-Calcination process. The Mn-doped alumina red pigment was tested by XRD, SEM and CIE L*a*b* colour parameter measurement. The results showed that the reaction of Mn(NO3)2·6H2O, Al(NO3)3·9H2O and CH3COONH4 with the theoretical ratio could be ignited and self-propagating at 500 °C. One kind pigment with excellent chromatic performance had been gained at the ratio about 1:40 between Mn(NO3)2·6H2O and Al(NO3)3·9H2O. The crystallite of the precursor obtained by Low-temperature Combustion synthesis (LCS) is imperfectly developed and the aggregation of particles is serious. The crystallite of the powder grows up more perfectly after calcined at 1000 °C for 4 hour with a corundum-like structure. The average particle size of the pigment is approximately 5 μm.