All five coordinating atoms of the amino-acid dianion L-aspartate (L-asp = NH2CH(COO)CH2COO2-) are found to be involved in coordination with Mnil in the presence of [Cr-III(CN)(6)](3-) to self-assemble into a chiral threedimensional cyanide-bridged K-3[Mn(L-asp)](6)[Cr(CN)(6)]center dot 2H(2)O containing the highest ratio of Mn:Cr of 6:1. It adopts the chiral P3 (no. 143) space group consisting of zigzag Mn-OCO-Mn chains sharing edges of hexagonal channels with central [Cr(CN)(6)](3-), while K+ and H2O occupy another parallel star-shaped channel. Its magnetic susceptibility above 100 K is dominated by the nearest neighbor (Mn-Cr at 5.08 and 5.31 antiferromagnetic (AF) exchange interactions (theta = -15(1) K) and below 40 K by further AF interaction between Mn and Mn at 5.32 angstrom. It finally reaches a steady value at 4.5 K, where a bifurcation of the zero-field-cooled and field-cooled magnetizations is observed in small fields (<1 kOe). The isothermal magnetization is linear in field and deviating toward saturation above 60 kOe at 2 K. No imaginary component of the ac susceptibilities is observed. This behavior is associated with long-range antiferromagnetic order of a helical or conic nature where the magnetic sublattices are numerous [2n X (6Mn + 1Cr)], leading to a domain of sufficient size to allow for the presence of the bifurcation. A model is proposed based on the local anisotropy and symmetry multiplicity of the space group.