Self-sensing and interfacial evaluation were investigated with different dispersion solvents for single carbon fiber/carbon nanotube (CNT)-epoxy composites by electro-micromechanical technique and acoustic emission (AE) under loading/subsequent unloading. Optimized dispersion procedure was set up to obtain improved mechanical and electrical properties. Apparent modulus and electrical contact resistivity for CNT-epoxy composites were correlated with different dispersion solvents for CNT. CNT-epoxy composites using good dispersion solvent showed higher apparent modulus because of better stress transferring effect due to relatively uniform dispersion of CNT in epoxy and enhanced interfacial adhesion between CNT and epoxy matrix. However, good solvent showed high apparent modulus but low thermodynamic work of adhesion, Wa for single carbon microfiber/CNT-epoxy composite. It is because hydrophobic high advanced contact angle was shown in good solvent, which can not be compatible with carbon microfiber well. Damage sensing was also detected simultaneously by AE combined with electrical resistance measurement. Electrical resistivity increased stepwise with progressing fiber fracture due to the maintaining numerous electrical contact by CNT.