Understanding how to develop highly efficient and robust adsorbents for the removal of organic dyes in wastewater is crucial in the face of the rapid development of industrialization. Herein, d-Ti3C2Txnanosheets (MXene) were combined with sodium alginate (SA), followed by electrospinning and successive Ca2+-mediated crosslinking, giving rise to a series of SA/MXene nanofiber membranes (NMs). The effects of the MXene content of the NMs on the adsorption performance for methylene blue (MB) were investigated systemically. Under the optimum MXene content of 0.74 wt.%, SA/MXene NMs possessed an MB adsorption capacity of 440 mg/g, which is much higher than SA/MXene beads with the same MXene content, pristine MXene, or electrospinning SA NMs. Furthermore, the optimum SA/MXene NMs showed excellent reusability. After the adsorbent was reused ten times, both the MB adsorption capacity and removal rate could remain at 95% of the levels found in the fresh samples, which indicates that the electrospinning technique has great potential for developing biomass-based adsorbents with high efficiency.