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Ba(CeSm)TiAlO (BCSTA, z = 0, 0.25, 0.50, 0.75, 1.00) ceramics sintered in nitrogen atmosphere were prepared by the conventional solid state reaction. The effects of Al substitution for Ti on microstructure and microwave dielectric properties in BCSTA ceramics have been investigated. X-ray diffraction spectra revealed only a single tungsten bronze in all the samples from z = 0 to z = 1.00 and backscatter electronic images confirmed a second BaAlTiO phase at z > 0.50. Besides, XPS results indicated that the incorporation of Al suppressed the reduction of Ti, which leaded to the microwave dielectric properties such as Q × f and τ value improvement in BCSTA ceramics. Typically, the optimum combination of microwave dielectric properties: Q × f ∼ 8401.76 GHz, ε ∼ 71.68, and τ ∼ +4.37 ppm/°C were obtained at z = 0.50 in BCSTA ceramics sintered in nitrogen atmosphere. [ABSTRACT FROM AUTHOR]