This study presents a novel signal amplification method for high-sensitive electrochemical immunosensing. Gold (Au)/N-trimethyl chitosan (TMC)/iron oxide (Fe3O4) (shell/shell/core) nanocomposite was used as a tracing tag to label antibody. The tag was shown to be capable of amplifying the recognition signal by high-density assembly of Au nanoparticles (NPs) on TMC/Fe3O4 particles. The remarkable conductivity of AuNPs provides a feasible pathway for electron transfer. The method was found to be simple, reliable and capable of high-sensitive detection of human serum albumin as a model, down to 0.2 pg/ml in the range of 0.25-1000 pg/ml. Findings of the present study would create new opportunities for sensitive and rapid detection of various analytes.