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.