Black phosphorus (BP) is a potential candidate for an anode in lithium ion batteries due to its high theoretical capacity and the large interlayer spacing in the monolayered phosphorene form, allowing for lithium intercalation/ deintercalation. In this study, large-scale exfoliation of bulk BP was accomplished using a solution of NaOH and N-methyl-2-pyrrolidone (NMP), yielding phosphorene, which can be assembled into nanoflakes using electrophoretic deposition (EPD). Through the systematic addition of NaOH and subsequent sonication, BP nanoflakes were obtained in high yields by EPD, allowing for the integration of these nanoflakes into an anode in the film state. Anodes with a charge/discharge capacity of 172 mAh/g at a rate of 200 mA/g were obtained, which are promising for battery applications through various post-film treatments.