In this study, a superficial and highly efficient hydrothermal synthesis method was developed for the in situ growth of amine-functionalized iron containing metal-organic frameworks (H2N-Fe-MIL-101 MOFs) on porous nickel foam (NicF) skeletons (H2N-Fe-MIL-101/NicF). The uniform decoration of the H2N-Fe-MIL-101 nanosheets thus generated on NicF was immobilized with follicle-stimulating hormone (FSH) antibody (Ab-FSH) to detect FSH antigen. In the present work, the Ab-FSH tagged H2N-Fe-MIL-101/NicF electrode was first applied as an immunosensor for the recognition of FSH, electrochemically. With all of the special characteristics, this material demonstrated superior specific recognition and sensitivity for FSH with an estimated detection limit (LOD) of 11.6 and 11.5 fg/mL for buffered and serum solutions, respectively. The availability of specific functional groups on MOFs makes them an interesting choice for exploring molecular sensing applications utilizing Ab-FSH tagged biomolecules.