Water contamination by heavy metals and dyes has been one of the most severe problems globally. Various techniques have been employed to remove these contaminants from water, including adsorption and photocatalysis, which are highly efficient and environmentally friendly approaches. The overuse of traditional petroleum-based plastics in the production of filtration systems aggravates the status quo due to negative impacts on the environment. Bio-based polysaccharide polymers with the green and benign features and potential for commercial applications have been employed as feasible alternatives to replace synthetic polymers and reduce environmental impacts. With unique chemical composition, molecular weights, and functional chemical groups such as hydroxyl, amine, and carboxyl groups, carbohydrate polymers show multitude potentials for dye and metal ion chelation. This review focused on the fabrication of carbohydrate polymers, such as chitosan, cellulose, alginate, pullulan, starch, and hyaluronic acid, into nanofibrous structures using the electrospinning method and their environmental applications.