La-Sr co-doped Ba1−x(La0.5Sr0.5)xCo2Fe16O27 (x = 0.0, 0.2, 0.4, 0.6, 0.8 and 1.0, respectively) hexaferrites were prepared by the solid-state method. W-type hexaferrite single phase structure with space group P63/mmc was obtained when the doping amount was x < 0.4 and an M-type hexaferrite and a spinel phase with smaller grains gradually replaced the W phase as the primary phases when x ≥ 0.6. The maximum Ms is 76.2 emu/g and the minimum Hc is 60 Oe at x = 0.4, as obtained by VSM analysis. The magnetoelectric properties of the samples were tested at 1–18 GHz with a vector network analyzer and the reflection loss was calculated based on transmission line theory. It was found that the introduction of an appropriate amount of La-Sr provides a large number of porosity defects while increasing the grain size, which can effectively improve the reflection of electromagnetic waves inside the material and dissipate more energy. At the same time, co-doping also makes the resonance frequency of the samples shift to lower frequency, resulting in tunable absorption properties in the C, X and Ku bands. When x = 0.2, the minimum reflection loss is −40.61 dB at 1.5 mm thickness, with the effective absorption bandwidth of 5.76 GHz in the X band; when x = 0.4, the minimum reflection loss is −37.45 dB at 2.5 mm, with the bandwidth of 4.97 GHz in the C band; when x = 0.6, the material has good absorption in both the X and Ku bands with the thickness less than 2 mm. The simple preparation method and good performance make La-Sr co-doped Co2W ferrite a promising microwave absorbing material.