We investigate the anisotropic magnetoelectric(ME) characteristics for the five-layer magnetization-graded multiferroic composites(MGMC). The magnetic anisotropy and corresponding anisotropic magnetomechanical effect, demagnetization effect and magneto-mechanical damping’s dependence on magnetic field direction result in an obvious anisotropic ME coupling effect. The experimental results show that ME voltage coefficient in H33 mode is remarkably larger than the other ones (H11, H31 and H13) over the whole Hdc range. Correspondingly, ∂VME/∂Hdc arrives about 420mV/Oe at an optimum bias magnetic field of 46Oe, which is approximately 40 times larger than that of the previous reported composite. Furthermore, it also demonstrates an obvious angular dependence on dc magnetic field. Taking advantage of these specifications, the MGMC can be used to detect weak dc magnetic field and its spatial orientation.