In order to improve the adhesion of the middle frequency magnetic sputtered zirconium coating on a polyurethane film, an anode layer source was used to pretreat the polyurethane film with nitrogen and oxygen ions. SEMs and AFM roughness profiles of treated samples and the contrast groups were obtained. Besides, XPS survey spectrums and high resolution spectrums were also investigated. The adhesion test revealed that ion bombardment could improve the adhesion to the polyurethane coating substrate. A better etching result of oxygen ions versus nitrogen predicts a higher bonding strength of zirconium coating on polyurethane and, indeed, the highest bonding strengths are for oxygen ion bombardment upto 13.3 MPa. As demonstrated in X-ray photoelectron spectroscopy, the oxygen ion also helps to introduce more active groups, and, therefore, it achieves a high value of adhesion strength.