Hybrid transition metal-based compounds show excellent performance in the field of enzyme-free glucose sensing. Herein, a one-step, green, facile, highly efficient microwave-assisted strategy for fabricating bimetallic Co/Zn metal–organic frameworks (denoted as ZIF67/ZIF8) is proposed. The structural characterization and phase investigation of ZIF67/ZIF8 are assessed by microscopically studies, elemental mapping, X-ray diffraction and X-ray photoelectron spectroscopy. The proportion of Co and Zn elements of ZIF67/ZIF8 has been elaborately regulated, resulting in enhanced electro-oxidation performance toward glucose compared to mono-metal organic frameworks. The synergy effect between Co and Zn proves to be crucial for optimizing electroanalytical ability, which endows outstanding glucose sensing performance, including high sensitivity of 833.61 μA/mM/cm2, wide linear range up to 5 mM and low detection limit to be 6.5 μM. Furthermore, to demonstrate the practical application capability of ZIF67/ZIF8, real-time analysis in human serum sample is conducted, which confirms its good anti-interference ability and recovery rate. With the advantages of low cost, ease of production and high environment tolerance, this work provides a versatile method to obtain non-noble metal based biosensing materials for non-enzymatic glucose detection.