In this paper, we report the nonlinear magnetoelectric response in a homogenous magnetostrictive/piezoelectric laminate material. The proposed magnetoelectric stack Fe73.5Cu1Nb3Si13.5B9/piezofiber is made up of high-permeability magnetostrictive Fe73.5Cu1Nb3Si13.5B9 foils and a piezoelectric Pb(Zr, Ti)O3 fiber composite. The time dependence of magnetoelectric interactions in the Fe73.5Cu1Nb3Si13.5B9/piezofiber structure driven by pulsed magnetic field was investigated in detail. The experimental results show that the magnetoelectric effect is strongly dependent on the external bias magnetic and pulsed magnetic field parameters. To detect the amplitude of a pulsed magnetic field, the output sensitivity reaches 17 mV/Oe, which is excited by a 100 μs width field. In addition, to measure the pulsed width, the output sensitivity reaches 5.4 mV/μs in the range of 0–300 μs. The results show that the proposed Fe73.5Cu1Nb3Si13.5B9/piezofiber sensor is ideally suited for pulsed magnetic field measurement.