Magnetoelectric(ME) coupling characteristics in multiferroic heterostructures with different thickness of nanocrystalline soft magnetic alloy has been investigated at low frequency. The ME response with obvious hysteresis, self-biased and dual-peak phenomenon is observed for multiferroic heterostructures, which results from strong magnetic interactions between two ferromagnetic materials with different magnetic properties, magnetostrictions and optimum bias magnetic fields H-dc,H-opti. The proposed multiferroic heterostructures not only enhance ME coupling significantly, but also broaden dc magnetic bias operating range and overcomes the limitations of narrow bias range. By optimizing the thickness of nanocrystalline soft magnetic alloy T-f, a significantly zero-biased ME voltage coefficient(MEVC) of 14.8mV/Oe (185 mV/cm.Oe) at T-f = 0.09 mm can be obtained, which is about 10.8 times as large as that of traditional PZT/Terfenol-D composite with a weak ME coupling at zero bias H-dc,H-zero. Furthermore, when T-f increases from 0.03 mm to 0.18 mm, the maximum MEVC increases nearly linearly with the increased T-f at H-dc,H-opti. Additionally, the experimental results demonstrate the ME response for multiferroic heterostructures spreads over a wide magnetic dc bias operating range. The excellent ME performance provides a promising and practicable application for both highly sensitive magnetic field sensors without bias and ME energy harvesters. (C) 2016 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.