For the fabrication of multifunctional biopolymer nanocomposites in the combination of carbon nanotubes (CNTs), recently increasing attention has been paid to an effective homogenization of CNTs within polymer matrices and a fine tuning of the concentration. We developed an efficient method to produce homogeneous CNT-polycaprolactone nanocomposites with various and controllable CNT concentrations using an ionically-modified multi-walled CNT, MWCNT-Cl. The modified MWCNTs could be homogeneously dispersed in tetrahydrofuran (THF). Polycaprolactone (PCL) as a biodegradable and biocompatible polymer was smoothly dissolved in the homogeneous MWCNT-Cl/THF solution without agglomeration of MWCNT-Cl. The physicochemical and mechanical properties of the resultant nanocomposites were examined and the biological usefulness was briefly assessed.