Marine fouling on concrete has become one of the severest problems that damage the surface and even cause internal corrosion of marine concrete. Dissimilarly to the previous abuse of toxic antifoulants, developing hydrophobic waterborne antifouling materials could be regarded as one of the most environment-friendly and potential directions to protect marine concrete. However, the insufficient hydrophobicity, antifouling, and mechanical properties limit their application. Herein, we reported a series of hybrid coatings combining hyperbranched polyglycerol (HPG) decorated waterborne fluoro silicone polyurethane (H) and HPG-grafted graphene oxide (G-HPG) that improve the hydrophobicity, antifouling, and mechanical properties. The hybrid materials were modified by the hyperbranched polyglycerol synthesized based on the anionic-ring-opening reaction between glycerol and ethylene glycol or polyethylene glycol. Remarkably, the hydrophobicity (115.19°) and antifouling properties (BSA absorption of 2.33 μg/cm2 and P. tricornutum attachment of 1.289 × 104 CFU/cm2) of the materials could be developed by the modification of HPG with higher generation numbers and backbone molecular weights. Moreover, the mechanical properties negligibly decreased (tensile strength decreased from 11.29 MPa to 10.49 MPa, same pencil hardness and adhesion grade as H of 2H and grade 2). The results revealed that the HPG of higher generation numbers and backbone molecular weights could benefit materials with enhanced antifouling properties and hydrophobicity. The method of hyperbranched modification can be regarded as potentially effective in developing the durability and antifouling properties of marine antifouling materials.