A novel strategy was proposed for preparing a highly sensitive glycoprotein sensor based on molecularly imprinted polymers (MIP), which was electropolymerized with o-phenylenediamine and 3-aminophenylboronic acid monohydrate in the presence of template molecules (bovine serum albumin (BSA)). Sensitivity improved dramatically owing to the application of a graphene-Au nanoparticles hybrid as the electrode modifier, and the immobilization of a large amount of 6-ferrocenylhexanethiol, as the electroactive species, onto nanoparticles. The quantification of BSA was realized by detecting the electrochemical oxidation signal of 6-ferrocenylhexanethiol, which was bonded onto the electrode. Under optimized conditions, a good relationship was obtained between the response current and logarithm of BSA concentration in the range of 1.0 × 10(-11) to 1.0 × 10(-5) g mL(-1) with a detection limit of 7.5 × 10(-12) g mL(-1) (S/N = 3). The resulting MIP sensor displayed good selectivity, reproducibility and stability.