  We show that low field magnetoelectric (ME) properties of helimagnets
Ba0.5Sr1.5Zn2(Fe1-xAlx)12O22 can be efficiently tailored by Al-substitution
level. As x increases, the critical magnetic field for switching electric
polarization is systematically reduced from ~1 T down to ~1 mT, and the ME
susceptibility is greatly enhanced to reach a giant value of 2.0 x 10^4 ps/m at
an optimum x = 0.08. We find that control of nontrivial orbital moment in the
octahedral Fe sites through the Al-substitution is crucial for fine tuning of
magnetic anisotropy and obtaining the conspicuously improved ME
characteristics.
