By means of density functional theory calculations, we systematically investigated the adsorption and diffusion properties of lithium ions on the armchair and zigzag phosphorene nanoribbons (AC-PNR and ZZ-PNR), in comparison with the pristine phosphorene. It is shown that both AC- and ZZ-PNR have a significantly enhanced Li binding strength but without sacrificing the Li mobility due to the presence of unique edge states. Besides, the ZZ-PNR with the width of 21.5 Å has a moderate working voltage (0.504–0.021 V), high capacity (541 mA h/g) and fast charge/discharge rate, which is more promising to be used as an anode material for LIBs. By contrast, the obvious depravation of the voltage is found in AC-PNR, which is mainly due to its weak stiffness that cannot afford the observed structural deformation during the lithiated process. Thus, it is highly expected to avoid the undesirable structural expansion in AC-PNR. The results presented here provide valuable insights into exploring high performance armchair/zigzag phosphorene nanoribbons for potential Li-ion battery applications.