High magnetization Fe3O4/OA-FeCo/Al2O3 nanocomposite magnetic clusters have been obtained using a modified oil-in-water miniemulsion method. These nanocomposite clusters dispersed in a ferrofluid carrier result in a magnetorheological fluid with improved characteristics. The magnetic clusters have a magnetic core consisting of a mixture of magnetite nanoparticles of about 6 nm average size, stabilized with oleic acid (Fe3O4/OA) and FeCo/Al2O3 particles of about 50 nm average size, compactly packed in the form of spherical clusters with a diameter distribution in the range 100-300 nm and a hydrophilic coating of sodium lauryl sulphate surfactant. The surface chemical composition of the Fe3O4/OA-FeCo/Al2O3 clusters investigated by XPS indicates the presence of the Co2+ and Co3+ oxidation states of cobalt and the components of Fe2+ and Fe3+ characteristic to both an enhanced oxidation state at the surface of the FeCo particles and to the presence of magnetic nanoparticles of spinel structure which are decorating the supporting FeCo. This specific decorating morphology is also indicated by TEM images. Advanced characterization of the Fe3O4/OA-FeCo/Al2O3 magnetic clusters has been performed using Mössbauer spectroscopy and magnetization measurements at various temperatures between 6 K and 200 K. The unexpected formation of Co ferrite decorating nanoparticles was supported by Mössbauer spectroscopy. The dispersion of magnetic clusters in the ferrofluid carrier highly influences the flow properties in the absence of the field (shear thinning for low and moderate shear rates) and especially in applied magnetic field, when significant magnetoviscous effect and shear thinning was observed for the whole range of shear rate values. Detailed analysis of the magnetorheological behavior of the nanocomposite magnetic clusters dispersed in a ferrofluid carrier evidence significantly higher normalized dynamic yield stress values in comparison with the magnetite nanocluster suspensions of the same mass concentration, a promising result for this new type of nanocomposite magnetorheological fluid.