The nitric oxide (NO) molecule has gained increasing attention in biological applications to combat biofilm-associated bacterial infections. However, limited NO loading, relatively short half-lives of low molecular weight NO donor compounds, and difficulties in targeted delivery of NO have hindered their practical clinical administration. To overcome these drawbacks, the combination of NO and scaffolds based on biocompatible polymers is an effective way towards realizing the practical utility of NO in biomedical applications. In this regard, the present overview highlights the recent developments in NO-releasing polymeric biomaterials for antimicrobial applications, focusing on antibiofilm treatments and the challenges that need to be overcome.