This article shows the success of using the chemical reduction method, the polyol thermolytic process, the sonochemistry method, and the hybrid sonochemistry/polyol process method to design iron-based magnetically active composite nanomaterials in a hyperbranched polyester polyol matrix. Four samples were obtained and characterized by transmission and scanning electron microscopy, infrared spectroscopy and thermogravimetry. In all cases, the hyperbranched polymer is an excellent stabilizer of the iron and iron oxides nanophase. In addition, during the thermolytic process and hybrid method, the branched polyol exhibits the properties of a good reducing agent. The use of various approaches to the synthesis of iron nanoparticles in a branched polyester polyol matrix makes it possible to control the composition, geometry, dispersity, and size of the iron-based nanophase and to create new promising materials with colloidal stability, low hemolytic activity, and good magnetic properties. The NMR relaxation method proved the possibility of using the obtained composites as tomographic probes.