The correlation between magnetic relaxation dynamics and the alignment of single-ion magnets (SIMs) in a crystal was investigated using four analogous cobalt(ii) complexes with unique hydrogen-bond networks. The hydrogen-bonding interactions in the crystals resulted in a relatively short intermolecular CoMIDLINE HORIZONTAL ELLIPSISCo distance, which led to non-zero intermolecular magnetic coupling. All the complexes with a CoMIDLINE HORIZONTAL ELLIPSISCo distance shorter than 6.5 angstrom exhibited zero-field slow magnetic relaxation as weak magnetic interactions split the ground +/- M-s levels and suppressed quantum tunneling of magnetization (QTM). In particular, antiferromagnetically coupled one-dimensional chain SIM networks effectively suppressed QTM when the two intrachain CoMIDLINE HORIZONTAL ELLIPSISCo distances were non-equivalent. However, when the two distances in a chain were equivalent and each molecular symmetry axis aligned parallell within the chain, QTM suppression was insufficient because magnetic coupling from the adjacent molecules was virtually cancelled. Partial substitution of the Co-II ion with the diamagnetic Zn-II ion up to 33% for this complex resulted in complete QTM suppression in the absence of an external field. These results show that the manipulation of intermolecular distances and alignments is effective for suppressing undesired QTM events in SIMs.