Multiferroic composites made by combining ferroelectric and ferromagnetic substances have been rapidly developed for their excellent magnetoelectric (ME) effect above room temperature, which ensures large potential applications in multifunctional devices, transducer, actuators, and sensors. [1][2][3] The magnetoelectric effect is characterized by the appearance of an electric polarization (ME H output) on applying a magnetic field or a magnetic polarization (ME E output) on applying an electric field. It is well known that the ME effect in the composites is a product property deriving form the coupling between a piezoelectric effect in the ferroelectric phase and a magnetostrictive effect in the ferromagnetic phase. [4,5] That is, when a magnetic field is applied to the composites, the ferromagnetic phase changes its shape magnetostrictively, and the strain is passed along to the piezoelectric phase, resulting in a change of electric polarization. Among bulk multiferroic composites, the composites containing giant magnetostrictive alloy Tb 1-x Dy x Fe 2 (Terfenol-D) and piezoelectric Pb(Zr,Ti)O 3 (PZT), exhibiting high magneto-and electromechanical energy densities, respectively, are the most attractive due to their giant ME response. [6][7][8] Using the concept of phase connectivity, [9] we can describe the structures of a two-phase composite by notations like 0-3, 2-2, and 1-3 etc., in which each number denotes the connectivity of the phase. So far, 0-3, 2-2, and 1-3 type structured composites containing Terfenol-D and PZT (especially 0-3 and 2-2 composites) have been widely investigated. For example, a threephase 0-3 type composite in which Terfenol-D particles (notated as 0) are dispersed in PZT/polymer matrix (notated as 3) has been developed. [10] Similarly, by using polymer as binder and matrix, the pseudo 2-2-type composites have been fabricated by stacking and easily hot-pressing the Terfenol-D/ polymer layer and PZT/polymer layer together.[11] The lowfrequency ME sensitivity of such 0-3 type and pseudo 2-2 type composites is about 100 mV cm -1 Oe order of magnitude. In particular, by directly gluing Terfenol-D and PZT plates together, a much stronger ME effect was observed in such 2-2 Terfenol-D/PZT laminated composites, and the ME coefficient can reach up to several V cm -1 Oe, [7,8] which is one order of magnitude larger than the former 0-3 and pseudo 2-2 type composites. But the brittleness and high eddy current loss at high frequency of Terfenol-D plates restrict their applications. Besides these 0-3 and 2-2 structures, the 1-3 structure, that is, a fiber (or rod) reinforced composite, is another important structure. Recently, such 1-3 structured composites with PZT rod arrays in a Terfenol-D/epoxy (TDE) medium have been reported, [12] and were fabricated via the same dice-and-fill procedure as for the well-known piezoelectric 1-3 composites, [13] to exhibit a high ME coefficient of about 6 V cm -1 Oe at resonance frequency. By the dice-and-fill procedure, the preparation of PZT rod arrays becomes ...