This study proposes a novel, cost‐effective nano CoFe2O4‐decorated halloysite nanotubes (CoFe2O4/HNT) catalyst, which effectively degrades the antibiotic ornidazole (ONZ) through peroxymonosulfate (PMS) activation. By using a simple and economical preparation method, ultra‐low amounts of CoFe2O4 are uniformly loaded onto HNTs, significantly improving the activity and stability of the catalyst. The experimental results show that the CoFe2O4/HNT+PMS system can almost completely degrade ONZ within 1 h, with good pH adaptability and resistance to anion interference. The simple synthesis process and low cost of CoFe2O4/HNT make it highly practical for large‐scale applications. Mechanism studies have shown that the synergistic effect between Co and Fe greatly improves the activation efficiency of PMS, generating reactive oxygen species (such as 1O2) that play a key role in ONZ degradation. This work not only elucidates the activation mechanism, but also provides insightful information for advanced oxidation processes (AOP). The results indicate the practicality and importance of CoFe2O4/HNT catalyst in treating harmful pollutants in water, supporting effective and sustainable water purification technologies. In addition, the study emphasizes the elasticity and adaptability of this innovative catalyst system in managing various pollutants, indicating its broad potential for environmental applications.