With less extra stress on the testing sample, a free-stress sample holder was designed to place the sample horizontally. With the free-stress sample holder, a magnetoelectric (ME) coefficient measurement system was developed based on dynamic method. This measurement system has the hardware part and the software part, integrated by the DC magnetic field generation module, the AC magnetic field generation module, the induced ME voltage detecting module and PC software module. Then, a sample of Terfenol-D/PZT/Terfenol-D trilayer was designed and fabricated, and the relationships of its ME coefficient influenced by the DC magnetic field and the frequency of the AC magnetic field were tested using the measurement system. And the results showed that the free-stress sample holder was proven to improve the accuracy of the measurement system by less stress interference.