Magnetic materials with highly efficient microwave absorption properties, crucial for dealing with the advanced wireless communications and radar detections, have been garnering significant attentions. Rare-earth transition-metal compounds were researched as the potential candidates but still suffer from the disadvantages of complex powder metallurgy process and low serving frequencies. In this work, the novel magnetic composites consisting of SmCo5 and Sm2Co17 are developed by a reduction diffusion method. The micromorphology and the binary phase ratios of the SmCo5/Sm2Co17 could be easily modulated by simply altering the reactant concentrations. Consequently, an optimum reflection loss of − 50.2 dB and broad absorption bandwidth of 4.95 GHz at a thickness of only 2.0 mm are achieved. The improved microwave absorption properties of the SmCo5/Sm2Co17 binary-phase magnetic absorbents can be attributed to their adjustable magnetic phases and the distinctive flaky particle shape, which greatly enhance microwave absorption capabilities. This work demonstrated a feasible reduction diffusion method and proposed a new strategy of designing binary-phase magnetic materials to achieve high microwave absorption properties.