We report a systematic study of the linear magnetoelectric effect in Co4Nb2O9 single crystals under pulsed magnetic fields up to 52 T. By applying sufficiently high magnetic and electric fields synergistically, a complete single-domain state is achieved, providing direct access to the intrinsic magnetoelectric response. Based on this, comprehensive field-dependent polarization measurements were performed along both Px (x//[110]) and Py (y//[1-10]) under various magnetic field orientations, yielding ΔPx ~1000 μC/m2 and ΔPy ~110 μC/m2, which allows determination of the full dominant linear magnetoelectric tensor components αxx, αxy, αyx, and αyy. The angular-dependent Px measurements reveal a periodic modulation of the linear magnetoelectric response in both multidomain and single-domain states, demonstrating that the polarization direction continuously follows the rotation of the magnetic moments under a rotating magnetic field.