The design and preparation of cheaper, greener and more efficient adsorbents is essential for the removal of pollutants by adsorption. In this study, biochar was prepared from peel of Brassica juncea var. gemmifera Lee et Lin (PoBJ) using a facile, low-temperature and vacuum pyrolysis, and the adsorption mechanism toward organic dyes in aqueous solution was elucidated. The adsorbent was characterized by XPS, FT-IR and SEM, and zeta potential techniques. The adsorption ability of PoBJ biochar for cationic dyes (methylene blue, brilliant green, calcein-safranine, azure I, rhodamine B), anionic dyes (alizarin yellow R), and neutral dyes (neutral red) revealed that the biochar exhibited adsorption selectivity toward cationic dyes. The effects of different factors on the adsorption performance of PoBJ biochar, as well as the adsorption kinetics and thermodynamics, were further investigated by using methylene blue as the model adsorbate. These factors included temperature, pH, contact time and dye concentration. The experimental results showed that BJ280 and BJ160 (prepared at 280 °C and 160 °C, respectively) possessed relatively higher adsorption capacity of 192.8 and 167.40 mg g−1 for methylene blue (MB), respectively, demonstrating the possibility of utilization of PoBJ biochar as a superior bio-adsorbent. The experimental data of BJ160 toward MB were correlated with various kinetic and isothermal models. The results indicated that the adsorption process was consistent with the Langmuir isotherm model and nonlinear pseudo-second-order kinetic model. Thermodynamic parameters indicated that the adsorption of MB onto BJ160 was exothermic. Thus, the low-temperature prepared PoBJ biochar was an environmentally friendly, economic and efficient cationic dye adsorbent.