Two kinds of two-dimensional (2D) covalent-organic frameworks (COF) were used to construct a sandwich-type electrochemical immunosensor for a proof-of-concept study. Vinyl-functionalized COFTab-Dva could be linked with Ab1 by the thiol–ene “click” reaction. Electroactive COFTFPB-Thi was modified with gold nanoparticles (AuNPs) to ensure the successful connection with Ab2 through Au–S bond. Meanwhile, electroactive COFTFPB-Thi was used to as signal probe to realize both the detection of carcinoembryonic antigen (CEA) and the amplification of detection signal. In detection process of the sandwich-type electrochemical immunosensor, glassy carbon electrode (GCE) was modified with 2D COFTab-Dva first then connected with Ab1 by the thiol–ene “click” reaction, next quantitative CEA was captured, followed by specificially capturing signal probe of Ab2/AuNPs/COFTFPB-Thi where AuNPs acted as nanocarriers of Ab2 and COFTFPB-Thi served as the signal producers. As the amount of CEA was increased, the amount of signal probe captured to the electrode was also increased, and the peak signal intensity of the redox reaction of COFTFPB-Thi was enhanced accordingly. Thus, the quantitative detection of CEA could be realized according to the peak signal intensity of electroactive COFTFPB-Thi. The electrochemical immunosensor owned wide detection range of 0.11 ng/mL-80 ng/mL, low detection limit of 0.034 ng/mL and good practicability. This study opens up a new revelation for quantitative detection of CEA using electroactive COF as enhanced signal probe.