The slight incommensurate modulation of the structure of Bi2Mn4/3Ni2/3O6 is sufficient to suppress the electrical polarization which arises in commensurate treatments of the structure, due to antiferroelectric coupling of local polar units of over 900 angstrom(3). The incommensurate structure is produced by the competition between ferroelectric Bi lone pair-driven A site displacement, chemical order of Mn and Ni on the B site, and both charge and orbital order at these transition metals. The interplay between the frustrated polar Bi displacements and the frustrated spin order at the B site, induced by positional disorder, produces magnetodielectric coupling between the incommensurately modulated lattice and the spin-glass-like ground state with an unusual relationship between the magnetocapacitance and the applied field.