In this paper, the flower-like FeCo/ZnO composites were successfully firstly prepared by a two-step method, and their microstructures and microwave absorbing properties were characterized. The results show that with an increase of temperature, the content of ZnO loaded on a FeCo/ZnO composite surface was increased. The optimal reflection loss (RL) value can be reached around −53.81 dB at 9.8 GHz, which is obviously superior to results of previous studies and reports, and its effective bandwidth (RL < −10 dB) is 3.8 GHz in the frequency range of 8.7–11.8 GHz with a matching thickness of 1.9 mm. We considered that a large number of lamellar and rod-like ZnO loaded on nano-FeCo single-phase solid solution by two-step method can significantly improve the electromagnetic wave absorption properties.