Magnetoelectric ceramic composites exhibit interesting physical properties for potential applications in multifunctional devices. These properties are affected by factors such as synthesis, processing, and connectivity of the constituent phases. Usually, the constituent phases are synthesized separately and mixed mechanically for conformation, which compromises the homogeneous distribution of the phases affecting negatively the magnetoelectric behavior, demanding a high energy consumption during the synthesis. In order to obtain a magnetoelectric nanocomposite with a homogeneous distribution of the phases and lower energy consumption in the synthesis process, this study reports the systematic results of the co-synthesized system (1-x)(Na0.5Bi0.5)0.94Ba0.06TiO3 - (x)CoFe2O4 (NBT-BT6/CFO) using the polymeric precursor synthesis method - Pechini. Different molar compositions of (1-x) NBT-BT6/CFO system, where x = 0.5, 0.3, and 0.2, were obtained at 700 °C for 1h. The morphological and structural analysis, carried out by XDR and SEM, techniques, showed the formation of the NBT-BT6/CFO nanocomposite in all study compositions with a highly homogeneous distribution among the phases. In addition, through magnetic hysteresis was verified an excellent magnetic behavior of all compositions. Thus, according to the results obtained, the composite is a promising material to present magnetoelectric properties.