The development of a simple yet novel aqueous solution based 'one-pot' method has been reported for the preparation of nanocomposites composed of soft ferrite (Mn0.2Ni0.4Zn0.4Fe2O4) and hard ferrite (BaFe12O19) phases. A physical mixing method has also been employed to prepare nanocomposites having the same compositions. The effects of synthetic methodologies on the microstructures of the nanocomposites as well as their magnetic and microwave absorption properties have been evaluated. The crystal structures and microstructures of these composites have been investigated using X-ray diffraction, transmission electron microscopy and scanning electron microscopy. In the nanocomposites prepared by both methods, the presence of nanocrystalline Mn0.2Ni0.4Zn0.4Fe2O4 and BaFe12O19 phases were detected. However, nanocomposites prepared by the one-pot method possessed better homogeneous distribution of hard and soft ferrite phases than the nanocomposites prepared by the physical mixing method. Very good spring exchange coupling interaction between the hard and soft ferrite phases was observed for the nanocomposites prepared by the one-pot method and these composites exhibited magnetically single phase behaviour. The spring exchange coupling interaction enhanced the magnetic properties (high saturation magnetization and coercivity) and microwave absorption properties of the nanocomposites prepared by the one-pot method, in comparison with the nanocomposites prepared by the physical mixing method as well as pure Mn0.2Ni0.4Zn0.4Fe2O4 and BaFe12O19 nanoparticles. The minimum reflection loss of the composites was found to be ∼-25 dB (i.e. >99% absorption) at 8.2 GHz with an absorber thickness of 3.5 mm. This journal is © the Partner Organisations 2014.