Graphene-based bionanocomposites are employed in several ailments, such as cancers and infectious diseases, due to their large surface area (to carry drugs), photothermal properties, and ease of their functionalization (owing to their active groups). Modification of graphene-derivatives with polysaccharides is a promising strategy to decrease their toxicity and improve target ability, which consequently enhances their biotherapeutic efficacy. Herein, functionalization of graphene-based materials with carbohydrate polymers (e.g., chitosan, starch, alginate, hyaluronic acid, and cellulose) are presented. Subsequently, recent advances in graphene nanomaterial/polysaccharide-based bionanocomposites in infection treatment and cancer therapy are comprehensively discussed. Pharmacogenomic and toxicity assessments for these bionanocomposites are also highlighted to provide insight for future optimized and smart investigations and researches.