The search for sustainable and efficient remediation techniques is required to control increasing environmental pollution caused by synthetic dyes, heavy metal ions, and other harmful pollutants. From this point of view, natural polymers like chitosan, cellulose, lignin, and pectin have been found highly promising due to their biodegradability, availability, and possibility of chemical functionalization. Natural polymers possess inherent adsorption properties that can be further enhanced by cross-linking and surface activation. This review discusses the main properties, adsorption mechanisms, and functional groups such as hydroxyl, carboxyl, and amino groups responsible for pollutant sequestration. The paper also emphasizes the effectiveness of natural polymers in removing heavy metals and dyes from wastewater and discusses recent advances in polymer modifications, including ionic crosslinking and grafting. This study underlines the ecological potential of natural polymer-based adsorbents in the treatment of wastewater and the protection of the environment as a sustainable solution to pollution challenges.