The treatment of heavy metal-contaminated water is challenging. The use of nanomaterials from many environmental wastes is promising for removing metals and contaminants from aqueous solutions. This study is novel in using nanobiochar of water hyacinth (WH) and black tea waste (TW) as a promising approach to water decontamination owing to its unique properties that play an effective role in metal adsorption. The mono- and multi-adsorption systems of cadmium (Cd), chromium (Cr), and nickel (Ni) on biochar and nanobiochar of water hyacinths (BWH and NBWH) and black tea waste (BTW and NBTW) were investigated in this study as potential low-cost and environmentally friendly absorbents for the removal of previously mentioned heavy metals (HMs) from aqueous solutions. The WH and TW were collected from the locality, prepared, and kept until used in the experiment. Nanobiochar was prepared by grinding, characterizing, and storing in airtight containers until used. A batch experiment was designed in mono- and competitive systems to study the adsorption equilibrium behavior of HMs on biochar and nanobiochars. The Freundlich and Langmuir isotherm models were fitted to the mono- and competitive-adsorption equilibrium results. The Freundlich isotherm model provided a better fit. Furthermore, it was noticed that NBWH and NBWT efficiently removed the Cd in the mono-system by ≥99.8, especially in the smaller concentration, while NBWT and BTW removed ≥99.8 and 99.7% in the competitive system, respectively. In the mono- and competitive systems, the nanobiochars of NBTW removed more than 98.8 of Cr. The sorbents were less efficient in Ni removal compared to Cd and Cr. However, their effectiveness was very high also. The results revealed that Cd was the highest metal removed by sorbents, nanobiochars were better than biochars to remove the HMs, and the results also indicated that co-occurrence of multi-metals might fully occupy the adsorption sites on biochars and nanobiochars.