Cross correlation between magnetism and electricity in a solid can host magnetoelectric effects, such as magnetic (electric) induction of polarization (magnetization). A key to attain the gigantic magnetoelectric response is to find the efficient magnetism–electricity coupling mechanisms. Among those, recently the emergence of spontaneous (ferroelectric) polarization in the insulating helimagnet or spiral-spin structure was unraveled, as mediated by the spin-exchange and spin–orbit interactions. The sign of the polarization depends on the helicity (spin rotation sense), while the polarization direction itself depends on further details of the mechanism and the underlying lattice symmetry. Here, we describe some prototypical examples of the spiral-spin multiferroics, which enable some unconventional magnetoelectric control such as the magnetic-field-induced change of the polarization direction and magnitude as well as the electric-field-induced change of the spin helicity and magnetic domain.