The engineering of a new type of trifunctional biopolymer-based
nanosponges polymerized by cross-linking beta-cyclodextrin ethylene
diamine (βCD–EDA) with bifunctional hairy nanocellulose
(BHNC) is reported herein. We refer to the highly cross-linked polymerized
BHNC−βCD–EDA network as BBE. βCD–EDA
and BHNC were cross-linked at various ratios with the help of DMTMM
(4-(4,6-dimethoxy-1,3,5-triazin-2-yl)-4-methylmorpholinium) as a green
activator in deionized water as a solvent, which resulted in different
morphological shapes of BBE. Some of these structures were chiral
due to cross-linked liquid crystalline structures. A comprehensive
characterization study was done to show their unique morphological,
structural, and dimensional properties of BBEs. Moreover, to further
investigate and to confirm the surface modification of the precursors
and final BBE structures, Fourier transform infrared and nuclear magnetic
resonance spectroscopy, thermogravimetric analysis, Brunauer–Emmett–Teller
analysis, and X-ray diffraction were applied. The hairy nanocellulose
particles were considered as the backbone, and the immobilized cyclodextrin
cavities can capture doxorubicin, which was used as a model drug molecule
via host–guest inclusion complexation. Finally, the obtained
BBE networks showed different and sustained drug release profiles
and pH responsiveness. BBE biopolymers were tested as biocompatible
nanocarriers for controlled release. We realize that these structures
are too big for anti-cancer drug delivery by injection or oral intake,
but these structures have a high potential to be applied in wound
dressing and implants. They could also be used for capturing antibiotics,
dyes, and organic compounds from wastewater.