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Nitric oxide (NO) has become one of the most studied molecules in the fascinating realm of the biomedical sciences over the last two decades, owing to its multifaceted role in a variety of physiological and pathophysiological processes. This has made the development of new strategies and methods for generating NO in a controlled fashion a hot topic in the burgeoning field of nanomedicine, with the exciting prospect to tackle important diseases. This paper illustrates very recent advances in the fabrication of multifunctional nanoconstructs which combine the photoregulated release of NO with additional fluorescence imaging and phototherapeutic modalities. Representative examples, including metal and supramolecular complexes, molecular conjugates, nanoparticles and thin films, will be described, highlighting the rationale design and their potential relevance in biomedical research.