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In this paper, we present a new method of using functionalized multi-walled carbon nanotubes (MWCNTs) to specifically detect anti-goat IgG. 3-Glycidoxypropyl-trimethoxysilane (GPTS) was immobilized onto the CNT surface to introduce epoxy ring and goat IgG was used as a biological probe. Afterwards, blockers were used to occupy the open space in the CNT surface, and finally anti-goat IgGs were detected by the functionalized MWCNTs. FSEM, AFM, TEM, and AT-FIR were used to characterize the physical and chemical property changes during each process. AFM results showed the CNT diameters increased accordingly as more immobilization processes were conducted. AT-FIR spectrum confirmed the success of biomolecules binding with CNTs in each process. The functionalized CNT for anti-goat IgG sensing was verified by another piezoelectric sensor. The functionalized MWCNTs could then be potentially used for immunosensor or incorporated with other sensors to enhance the sensitivity.