The bond strength and stability of the intermolecular network structure of cellulose play a decisive role in the tensile strength and rupture resistance of paper. In this work, the surface morphology, the chemical composition, and the crystal structure of nanocellulose prepared from cotton fibers were characterized by scanning electron microscopy (SEM) analysis, X-ray diffraction (XRD), and Fourier transform infrared spectroscopy (FTIR) to prepare cotton fiber nanocellulose by green solvent deep-eutectic solvent pretreatment combined with the ultrasonic method. Nanocellulose of different morphology and structure was used as a papermaking additive to explore its effect on the strength performance of the paper. The results show that the burst resistance index of the paper handsheets could be increased by 6.1% and 9.8%. The burst resistance index improved as the added amount of the NFC was increased.