“…Biomolecule-induced colloidal assembly plays an increasingly important role in biomedical applications due to the integration of unique physiochemical properties of nanoparticles (NPs) and bio-functions of proteins, enzymes, and DNA. − Among them, aggregates from the building block of magnetic nanocrystals functionalized with the protein corona exhibited high potential as a pivotal tool for both fundamental research and application-oriented research, such as biodetection and tissue engineering. − The ability to manipulate the anisotropic self-assembly of a colloidal system in the presence of protein has opened up an emerging route toward the development of smart materials with designable properties. , To date, a majority of colloidal assemblies with a threadlike morphology based on the magnetic NPs have been frequently realized through one of the typical external stimuli magnetic forces in a solution environment, in which the NP can be aligned along the magnetic force lines. − Instead, for tuning the anisotropic self-assembly behavior of small-size gold NPs and iron oxide nanocrystals, several categories of molecular interactions involving the interplay of anisotropic dipolar forces, electrostatic interaction, hydrophobic interaction, intramolecular hydrogen bonds, and isotropic van der Waals forces have been studied in the past decade. − So far, there has been no report to identify the effect of the functionalized NP–protein interaction and protein intermolecular interaction on the robust anisotropic self-assembly of magnetic nanospheres to form tens of microns anisotropic colloidal assembly (TMACA).…”