The itinerant electron density (n) near the Fermi level has a close correlation with the physical properties of Sr 2 FeMoO 6 . Two series of single-phase Sr (2Ày) Na y FeMoO 6 (y ¼ 0.1, 0.2, 0.3) and Sr (2Ày) Na y Fe (1Àx) Mo (1+x) O 6 (y ¼ 2x; y ¼ 0.1, 0.2, 0.3) ceramics were specially designed and the itinerant electron density (n) of them can be artificially controlled to be: n ¼ 1 À y and n ¼ 1 À y + 3x ¼ 1 + 0.5y, respectively. The corresponding crystal structure, magnetization and the ferromagnetic Curie temperature (T C ) of two subjects were investigated systematically. The X-ray diffraction analysis indicates that Sr (2Ày) Na y behavior confirms that it is the Fe/Mo ASD not n that dominantly determines the magnetization properties. Interestingly, approximately when n # 0.9, T C of Sr (2Ày) Na y FeMoO 6 (y ¼ 0.1, 0.2, 0.3) exhibits an overall increase with decreasing n, which is contrary to the T C response in electron-doped SFMO.Such abnormal T C is supposed to relate with the ratio variation of n(Mo)/n(Fe). Moreover, when n $ 1, T C of Sr (2Ày) Na y Fe (1Àx) Mo (1+x) O 6 (y ¼ 2x; y ¼ 0.3) exhibits a considerable rise of about 75 K over that of Sr (2Ày) Na y Fe (1Àx) Mo (1+x) O 6 (y ¼ 2x; y ¼ 0.1), resulting from improved n caused by introducing excess Mo into Sr (2Ày) Na y FeMoO 6 . Maybe, our work can provide an effective strategy to artificially control n and ferromagnetic T C accordingly, and provoke further investigation on the FeMo-baseddouble perovskites.