Multiferroic materials have attracted much attention because of their magnetoelectric coupling effect. In this paper, MnFe2O4 (MFO) magnetic particles and PbZr0.52Ti0.48O3 (PZT) ferroelectric particles were prepared by hydrothermal method and sol-gel method, respectively. PZT particles with different sizes were produced by tuning the sintering temperature, and on this basis, MFO-PZT multiferroic liquid was prepared by using monoamino ethoxy-coupling agent as the surfactants and dimethyl silicone oil as the carrier liquid. The effect of PZT particle size on magnetoelectric properties was studied. XRD and SEM show that the PZT particle and the MFO particle have no secondary phase, the size of MFO particle is 52 nm, and the PZT particle sizes are 0.38 mu m, 1.07 mu m, 1.68 mu m, and 1.79 mu m, respectively. When the particle size of PZT is 0.38 mu m, a large dielectric constant of 8.39 of the multiferroic liquid was observed at low frequency (250 Hz). When the size of PZT is 1.79 mu m, the liquid has the maximum saturation polarization intensity P-s similar to 0.0191 mu C/cm(2) and the maximum residual polarization intensity P-r similar to 0.0063 mu C/cm(2) was obtained. When a magnetic field is applied, the value of both P-r and P-s increases. When the size of PZT is 1.07 mu m, the maximum magnetoelectric coupling coefficient of the liquid is 54.82 V /(cm.Oe). Compared with the same series of magnetoelectric materials, the magnetoelectric composite multiferroic liquid has a potential application prospect.