Nanotechnology has been widely used for developing sensors with higher sensitivity and better selectivity. In this study, a molecularly imprinted electrochemical sensor based on nitrogen-doped carbon nanosheet frameworks decorated with Fe (Fe-NCNF) was proposed for simultaneous detection of mebendazole (Meb) and catechol (CC). Fe-NCNF was prepared by chemical blowing, and it was coated with molecularly imprinted polymer (MIP) to construct a novel hybrid nanomaterial, which is named Fe-NCNF/MIP. Meb-MIP was electro-polymerized with methacrylic acid (MAA) as monomer via cyclic voltammetry (CV) method. This sensor architecture can detect Meb because of the high binding affinity of MIP. With the large specific surface area, Fe-NCNF can adsorb and electrochemically oxidize CC. The good selectivity of Fe-NCNF/MIP for CC and Meb was proven by anti-interference test, for which the oxidation potentials were set at 0.15 and 0.82 V respectively. The linear range for determination of CC was from 0.5 to 25 mu M with a low limit of detection (LOD) of 0.06 mu M (S/N = 3), and that for Meb was 0.01-1.5 mu M with a low LOD of 0.004 mu M (S/N = 3). Furthermore, this MIP electrochemical sensor was applied for the simultaneous detection of CC and Meb in tap water and river water. These results demonstrated that this method is reliable for selective, sensitive and feasible determination of Meb and CC.