Effect of iteration times on mechanically-activated combustion synthesis of high α-content Si3N4 powders was investigated. Properties of the as-synthesized powders such as α-content (Cα) as well as specific surface area (As) were examined. Results showed that both of Cα and As became higher after iteration reactions. The mechanical properties of the sintered bulk ceramics from as-synthesized powders were also tested to reveal the sinterability of the powders. Results showed that relative density of all the sintered bulk ceramics were higher than 97%. Furthermore, fracture toughness had a trend of becoming higher, which reached a value of 10.2 MPam0.5. Correspondingly, bending strenth became a bit lower.