Well‐Defined Protein‐Based Supramolecular Nanoparticles with Excellent MRI Abilities for Multifunctional Delivery Systems

Protein‐based nanoparticles are widely used for effective biomedical applications. The objective of this work is to design series of magnetic resonance imaging (MRI)‐visible cationic supramolecular nanoparticles (PGEA@BSA‐Ad/Gd3+) based on bovine serum albumin (BSA) and β‐cyclodextrin‐cored star ethanolamine‐functionalized poly(glycidyl methacrylate) (CD‐PGEA) in the presence of Gd3+ ions for multifunctional delivery systems. CD‐PGEA is prepared via atom transfer radical polymerization and ring‐opening reaction. It is found that in the absence of Gd3+ ions, CD‐PGEA does not well interact with adamantine‐modified BSA (BSA‐Ad). The well‐defined PGEA@BSA‐Ad/Gd3+ supramolecular nanoparticles could be produced through the synergistic actions of the host–guest and electrostatic self‐assemblies by mixing aqueous solutions of CD‐PGEA, BSA‐Ad, and Gd3+. In comparison with CD‐PGEA assembly units, such kinds of uniform PGEA@BSA‐Ad/Gd3+ supramolecular nanoparticles exhibit better pDNA condensation ability, lower cytotoxicity, higher gene transfection, and easier cellular uptake. In addition, PGEA@BSA‐Ad/Gd3+ also produces outstanding MRI abilities, much better than Magnevist (Gd‐diethylenetriaminepentacetate acid). The present design of protein–polymer supramolecular nanoparticles with MRI contrast agents would provide a new way for multifunctional gene/drug delivery systems.