In this work multiwalled carbon nanotube (MWCNT)/fibrin hybrid structures were synthesized via the transglutaminase- catalyzed polymerization of fibrinogen (FBG). Specifically, FBG was tethered onto oxidized MWCNTs by amide coupling, and the in situ polymerization of FBG to fibrin was performed by plasma transglutaminase (Factor XIIIa) in the presence of thrombin. The attached FBG was found to be biologically active and was polymerized to fibrin by thrombin and Factor XIIIa. MWCNT-FBG and MWCNT-Fibrin structures were characterized by FT-IR spectroscopy, transmission electron microscopy, and energy-dispersive X-ray (EDX) spectroscopy.