It is highly desirable to develop a safe, highly efficient, and biodegradable drug carrier with an enhanced drug transport efficiency. Cellulose nanofibrils (CNF) and chitosan (CS) composite hydrogels are promising candidate carriers with biological compatibility and non-cytotoxicity. Herein, the CNF/CS composite beads were prepared by dissolving cellulose and CS in LiBr molten salt hydrate and regenerating in ethanol. This preparation method is facile and efficient, and the obtained porous CNF/CS beads with the weight ratio of 8:2 exhibited a large specific surface area, uniform micro-nano-sized pores, strong mechanical property, and water absorption-resistance. Moreover, these beads as drug (tetracycline hydrochloride, TH) carriers showed a higher encapsulation efficiency (47.4%) at the TH concentration of 5 mg/mL in 24 h, and a higher drug loading rate (12.0%) than pure CNF and other CNF/CS beads prepared with different ratios. In addition, the TH releasing behavior of CNF/CS (8:2) beads fitted well into the zero-order, first-order, and Higuchi models under an acid condition, indicating that the drug release of these pH-sensitive beads was mainly affected by drug concentration under an acid condition. Therefore, these CNF/CS beads have great potential to be used as drug carriers for medical applications.