Ferroelectric/ferromagnetic composites (FFC) have attracted increasing attention because of their ferroelectric and magnetic properties. [1][2][3][4][5] They can be used to produce inductancecapacitance integrated filters, [6,7] which will reduce the space occupied on circuit boards and promote integration and miniaturization. [8] However, the capacitance (inductance) reduces with reducing the ferroelectric (ferromagnetic) phase fraction according to the compound law. Therefore, it is hard to obtain both high capacitance and high inductance from general FFCs. It is well known that the dielectric properties may be distinctly increased through the percolation effect near the percolation threshold. [8][9][10][11][12][13][14] However, the universal percolation threshold is very low (< 0.2). Even though we have prepared a percolative FFC with comparatively high percolation threshold (about 0.5) and high dielectric properties (about 10 times higher than that of the original perovskite phase) by the conventional ceramic method (CCM), [4] the percolation threshold (the content of ferrite phase) was not high enough and the permeability was only 20 % of pure magnetic ferrite. Therefore, the content of the ferrite phase should be significantly increased while the ferrite particles are prevented from connecting with each other. These requirements seems very hard to achieve by CCM. [4,[8][9][10][11][12][13][14][15][16] Therefore, it is of great importance to find a new method to produce the ferrite well surrounded by only a thin perovskite layer, which can avoid connection among the ferrite particles. If this can be achieved, on the one hand, the percolation threshold and thus the permeability of the FFCs can be increased, and, on the other hand, the permittivity can be increased significantly owing to the thinner perovskite layer. It is well known that molecular scale homogeneity can be ideally realized by sol-gel processes, and consequently homogeneous dispersions of components in composites can be obtained. In addition, the sol-gel method can be used for in situ formation of two phases, either alternately arranged or homogeneously dispersed as a two-phase system. A high threshold system with a high content and low connection of the conductive phase would likely be formed in this way.Herein, we propose two typical biphasic systems and a sol-gel preparation method, as well as an in situ multiphase formation process. The first system is PbTiO 3 (PTO)/NiFe 2 O 4 (NFO). The second is BaTiO 3 (BTO)/Ni 0.5 Zn 0.5 Fe 2 O 4 (NZFO). It is worth noting that PTO and BTO are typical ferroelectric phases with low conductivity (s % 10 À10 S cm À1 ), and NFO and NZFO are typical ferrimagnetic phases with comparatively high conductivity (s % 10 À3 S cm À1 ) and are suitable for percolating conditions.In this work, homogenously dispersed multiphase composites with extremely high content of ferrimagnetic phases were formed in situ by sol-gel processes. Typical XRD patterns of the PTO/NFO and BTO/NZFO ceramic composites (Figure 1) exhibit pea...