Nitric oxide (NO) serves a multitude of functions in human physiology and pathology, and therapeutic NO-releasing materials are vigorously developed for biomedical applications. Owing to its complex functions and its potential systemic effects, controllable NO release is desired for clinical applications. This review summarizes recent developments in the last five years in designing controllable NO-delivering platforms for treating diseases such as cancer, bacterial infection, cardiovascular diseases, wounds, and eye diseases, with a focus on the most commonly used NO donors, including N-diazeniumdiolates, S-nitrosothiols, arginine, and N-nitrosoamines. The progress and success of NO delivery strategies are highlighted, and their limitations are also included. Moreover, the therapeutic mechanisms of NO in the diseases are summarized, along with the corresponding means of controlling NO release. Finally, the prospects and potential challenges regarding the development of NO gas therapy are described, with the hope of encouraging new research in this area.