In this work, we develop a mussel-inspired biosorbent combined with graphene oxide for removal of organic dyes in water sources. The composite was prepared via self-polymerization of dopamine in weak alkaline solution containing graphene oxide at ambient condition. Morphological and structural studies revealed that polydopamine has gradually grown to cover the surface of graphene oxide flakes, partially reduced these flakes, and somehow form many grains (size around 20 nm) on the flakes instead of making very large aggregates as usual. The mass ratio between two components of the composite was also investigated to find the optimal one which provides enough surface area (20 m².g⁻¹) and maintain adhesive sites in order to ensure high-efficiency removal of organic molecules. The adsorption kinetics and isotherms of as-prepared adsorbent towards methylene blue were found to fit well with pseudo-first order kinetics model and Langmuir isotherm. The maximum adsorption capacity (q_m) and Langmuir constant (k_L) were estimated to be 270 mg.g⁻¹ and 0.49 L. mg⁻¹. The as-prepared bio-sorbent is very promising for remediation of water sources contaminated with cationic organic molecules and heavy metal ions.