Contaminants in water bodies cause potential health risks for humans and great environmental threats. Therefore, the development and exploration of low-cost, promising adsorbents to remove contaminants from water resources as a sustainable option is one focus of the scientific community. Here, we conducted a critical review regarding the application of pristine and modified/treated biosorbents derived from leaves for the removal of various contaminants. These include potentially toxic cationic and oxyanionic metal ions, radioactive metal ions, rare earth elements, organic cationic and anionic dyes, phosphate, ammonium, and fluoride from water media. Similar to lignocellulose-based biosorbents, leaf-based biosorbents exhibit a low specific surface area and total pore volume but have abundant surface functional groups, high concentrations of light metals, and a high net surface charge density. The maximum adsorption capacity of biosorbents strongly depends on the operation conditions, experiment types, and adsorbate nature. The absorption mechanism of contaminants onto biosorbents is complex; therefore, typical experiments used to identify the primary mechanism of the adsorption of contaminants onto biosorbents were thoroughly discussed. It was concluded that byproduct leaves are renewable, biodegradable, and promising biosorbents which have the potential to be used as a low-cost green alternative to commercial activated carbon for effective removal of various contaminants from the water environment in the real-scale plants.