This research introduces an innovative approach for evaluating the degree of densification of carbon nanotube (CNT) sheets produced through direct spinning and subsequently treated with organic solvent (specifically ethanol). Analysis of the morphological features of the CNT sheets from the FE-SEM image affirms that the sheet’s structure becomes more densified following the treatment. Based on this, the treated CNT sheet was comprehensively evaluated using Raman spectroscopy. The results indicate a downward shift in the G′ band, signifying the densification of the CNT sheet’s structure due to the C–C bond weakening by the cohesive force. Following ethanol treatment, the CNT sheet exhibited enhanced electrical conductivity and tensile strength, measuring approximately 1.7 × 105 S m− 1 and 138.7 MPa, respectively, a remarkable improvement of roughly 300% compared to the untreated CNT sheet. This study underscores the efficacy of Raman spectroscopy as a powerful tool for assessing the densification of CNT sheets.