Controlled self-assembly of inorganic nanoparticles has the potential to generate complex nanostructures with distinctive properties. The advancement of more precise techniques empowers researchers in constructing and assembling diverse building blocks, marking a pivotal evolution in nanotechnology and biomedicine. This progress enables the creation of customizable biomaterials with unique characteristics and functions. This comprehensive review takes an innovative approach to explore the current state-of-the-art self-assembly methods and the key interactions driving the self-assembly processes and provides a range of examples of biomedical and therapeutic applications involving inorganic or hybrid nanoparticles and structures. Self-assembly methods applied to bionanomaterials are presented, ranging from commonly used methods in cancer phototherapy and drug delivery to emerging techniques in bioimaging and tissue engineering. The most promising and experimental results achieved thus far are presented. Additionally, the review engages in a discourse on safety and biocompatibility concerns related to inorganic self-assembled nanomaterials. Finally, opinions on future challenges and prospects anticipated in this evolving field are provided.
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