Palladium (Pd) is widely used in catalyst, aerospace, and medical applications, but only 1% of its reserves are found in nature. So, the recovery of Pd(II) is very important. Natural fibers are a good adsorption material, and the abundant functional groups in bamboo shoot shell (BSS) fibers can form interactions with metal particles. However, few studies on Pd(II) adsorption using BSS fibers exist. In the present work, waste bamboo shoot shells were doped with titanium dioxide (TiO2) particles, and the surface activation of BSS-TiO2@CA by citric acid (CA) was carried out to prepare an efficient and recyclable adsorbent BSS-TiO2@CA for the adsorption of Pd(II). The adsorption performance, adsorption mechanism, and regeneration performance of BSS-TiO2@CA on Pd(II) were systematically analyzed by continuous adsorption experiments, characterization, and response surface method. It was found that the surface-activated waste bamboo shoot shells had an outstanding adsorption capacity of Pd(II), and the maximum adsorption rate of BSS-TiO2@CA reached 85% with a maximum adsorption capacity (Qm) of 175.74 mg/g. The functionalized use of waste bamboo shoot shells provides a new idea for the development of sustainable, cost-effective, and environmentally friendly adsorbents.