AbstractMultiferroics materials, which exhibit coupled magnetic and ferroelectric properties, have attracted tremendous research interest because of their potential in constructing next-generation multifunctional devices. The application of single-phase multiferroics is currently limited by their usually small magnetoelectric effects. Here, we report the realization of giant magnetoelectric effects in a Y-type hexaferrite Ba_0.4Sr_1.6Mg₂Fe₁₂O₂₂ single crystal, which exhibits record-breaking direct and converse magnetoelectric coefficients and a large electric-field-reversed magnetization. We have uncovered the origin of the giant magnetoelectric effects by a systematic study in the Ba_2-x Sr _x Mg₂Fe₁₂O₂₂ family with magnetization, ferroelectricity and neutron diffraction measurements. With the transverse spin cone symmetry restricted to be two-fold, the one-step sharp magnetization reversal is realized and giant magnetoelectric coefficients are achieved. Our study reveals that tuning magnetic symmetry is an effective route to enhance the magnetoelectric effects also in multiferroic hexaferrites.