Recent studies support that magnetic chiral nanozymes, integrating the features of chirality, magnetism, and enzyme-like catalysis, provide new insights into the synthetic methodologies and applications of chiral nanozymes. In this study, we present the design of novel magnetic chiral cobalt superstructures (CoSSs) synthesized by the regulation of complex formation kinetics of Co³⁺ with chiral ligands (L- or D-tartaric acid) under varying metal-to-ligand molar ratios and solvent polarity. This approach yielded a series of CoSSs with varying symmetry from high to low. The chiral CoSSs exhibited chirality-dependent peroxidase (POD)-like activity, demonstrating a high affinity of L-CoSSs towards substrates, with a chiral selective factor of approximately 1.37. In addition, the magneto-optical effects of the chiral CoSSs significantly enhanced their chiroptical performance from ultraviolet–visible (UV–vis) to near-infrared region. Under a magnetic field, the affinity of chiral CoSSs for substrates increases, while the chiral selective factor was modified to 0.76. This research on magnetic chiral CoSSs nanozymes opens promising new avenues for the application of artificial enzymes in fields, such as antibacterial technology, drug delivery, and biocatalysis.