We report the exceptional observation of two different magnetic ground states (MGS), spin glass (SG, T-B = 7 K) and ferrimagnet (FI, T-C = 18 K), for one crystal structure of [{Mn-II(D/L-NH(2)ala)}(3){Mn-III(CN)(6)}]center dot 3H(2)O obtained from [Mn(CN)(6)](3-) and D/L-aminoalanine, in contrast to one MGS for [{Mn-II(L-NH(2)ala)}(3){Cr-III(CN)(6)}]center dot 3H(2)O. They consist of three Mn(NH(2)ala) helical chains bridged by M-III(CN)(6) to give the framework with disordered water molecules in channels and between the M-III(CN)(6). Both MGS are characterized by a negative Weiss constant, bifurcation in ZFC-FC magnetizations, blocking of the moments, both components of the ac susceptibilities, and hysteresis. They differ in the critical temperatures, absolute magnetization for 5 Oe FC (lack of spontaneous magnetization for the SG), and the shapes of the hysteresis and coercive fields. While isotropic pressure increases both T-crit and the magnetizations linearly and reversibly in each case, dehydration progressively transforms the FI into the SG as followed by concerted in situ magnetic measurements and single-crystal diffraction. The relative strengths of the two moderate Mn-III-CN-Mn-II antiferromagnetic (J(1) and J(2)), the weak Mn-II-OCO-Mn-II (J(3)), and Dzyaloshinkii-Moriya antisymmetric (DM) interactions generate the two sets of characters. Examination of the bond lengths and angles for several crystals and their corresponding magnetic properties reveals a correlation between the distortion of Mn-III(CN)(6) and the MGS. SG is favored by higher magnetic anisotropy by less distorted Mn-III(CN)(6) in good accordance with the Mn-Cr system. This conclusion is also born out of the magnetization measurements on orientated single crystals with fields parallel and perpendicular to the unique c axis of the hexagonal space group.