A solution combustion process for the synthesis of hollandite (BaAl2Ti6O16) powders is described. SYNROC (synthetic rock) consists of four main titanate phases: perovskite, zirconolite, hollandite and rutile. Hollandite is one of the crystalline host matrices used for the disposal of high-level radioactive wastes because it immobilizes Sr and Lns elements by forming solid solutions. The solution combustion synthesis, which is a self-sustaining oxi-reduction reaction between a nitrate and organic fuel, generates an exothermic reaction and that heat converts the precursors into their corresponding oxide products in air. The process has high energy efficiency, fast heating rates, short reaction times, and high compositional homogeneity. To confirm the combustion synthesis reaction, FT-IR analysis was conducted using glycine with a carboxyl group and an amine as fuel to observe its bonding with metal element in the nitrate. TG-DTA, X-ray diffraction analysis, SEM and EDS were performed to confirm the formed phases and morphology. Powders with an uncontrolled shape were obtained through a general oxide-route process, confirming hollandite powders with micro-sized soft agglomerates consisting of nano-sized primary particles can be prepared using these methods.