In order to prepare microwave-absorbing materials with low density and high wave absorption performance, CoFe2O4/SWCNTs composites with well-designed necklace-like structures were successfully prepared in this paper by a simple solvothermal method. CoFe2O4/SWCNTs composites with different cobalt salt contents were synthesized by adjusting the experimental parameters. The results of the relative complex permeability and relative permittivity of the samples, which were investigated by vector network analysis in the frequency range of 2 to 18 GHz, are collected to support the study of the microwave absorption characteristics of the samples. Different microsphere densities and different cobalt salt contents have obvious differences in the electromagnetic absorption properties of the composites. When the additions of FeCl3·6H2O, Co(Ac)2·4H2O, and NH4Ac were 0.432, 0.200, and 0.400 g, respectively, the best reflection loss reached −42.07 dB, and the effective absorption frequency (RL < −10 dB) ranges from 3.2 to 18 GHz. Therefore, this is a preparation strategy of CoFe2O4/SWCNTs composites with necklace structure, which has the advantages of simple process, environmental friendliness, low cost, and high stability. The unique necklace-like structure design makes the carbon nanotubes partially exposed, which is more beneficial to achieve good impedance matching and giving the CoFe2O4/SWCNTs composite excellent electromagnetic loss capability.