Neodymium (Nd)-substituted cobalt ferrite nanoparticles (NPs), i.e., CoNdxFe2−xO4 (0.0 ≤ x ≤ 0.2) NPs, were synthesized by the sonochemical method. The compositional characterization was done by scanning electron microscopy (SEM) equipped with energy-dispersive X-ray spectroscopy (EDX) and transmission electron microscopy (TEM). Antistaphylococcal activity was found to be enhanced, i.e., survival rate was 50%, 45%, 40%, and 30% with the increase in the ratio of Nd (0.0 ≤ x ≤ 0.2), whereas anticandidal activity was found efficient, i.e., 9%, 20%, 22%, and 40% survival rate at all the four ratios. The morphogenesis studies indicated that the synthesized metal–ligand, improves the antimicrobial capacity by binding them strongly to the microbial walls. To the best of our knowledge, this is the first report which demonstrates the series of CoNdxFe2−xO4 (0.0 ≤ x ≤ 0.2) NPs being active towards Staphylococcus aureus and Candida albicans and encourages its potential candidature for pharmaceutical and biomedical purposes.