Fe powders with elongated and aggregated structure as heat pellet material for thermal battery applications were prepared by spray pyrolysis under various preparation conditions. The precursor powders with spherical shapes and hollow morphologies turned into Fe powders after reduction at a temperature of 615˚C under 20% H2/Ar gas. The powders had pure Fe crystal structures irrespective of the preparation conditions of the precursor powders in the spray pyrolysis. The morphologies and mean sizes of the Fe powders are affected by the preparation conditions of the precursor powders in the spray pyrolysis. Therefore, the ignition sensitivities and the burn rates of the heat pellets formed from the Fe powders prepared by spray pyrolysis are affected by the preparations of the precursor powders. The Fe powders prepared under the optimum preparation conditions have a BET surface area of 2.9 m2g1. The heat pellets prepared from the Fe powders with elongated and aggregated structure have a good ignition sensitivity of 1.1W and a high burn rate of 18 cms1.