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Carbon nanotube (CNT) thin sheet, or buckypaper, has shown great potential as a multifunctional platform material due to its desirable properties, including its lightweight nature, high mechanical properties, and good conductivity. However, their mass adoption and applications by industry have run into significant bottlenecks because of large variability and uncertainty in quality during fabrication. There is an urgent demand to produce high-quality, high-performance buckypaper at an industrial scale. Raman spectroscopy provides detailed nanostructure information within seconds, and the obtained spectra can be decomposed into multiple effects associated with diverse quality characteristics of buckypaper. However, the decomposed effects are high-dimensional, and a systematic quantification method for buckypaper quality assessment has been lacking. In this paper, we propose a real-time data-driven quality assessment method, which fills in the blank of quantifying the quality for continuous manufacturing processes of CNT buckypaper. The composite indices derived from the proposed method are developed by analyzing in-line Raman spectroscopy sensing data. Weighted cross-correlation and maximum margin clustering are used to fuse the fixed effects into an inconsistency index to monitor the long-term mean shift of the process and to fuse the normal effects into a uniformity index to monitor the within-sample normality. Those individual quality indices are then combined into a composite index to reflect the overall quality of buckypaper. A case study indicates that our proposed approach can determine the quality rank for ten samples, and can provide quantitative quality indices for single-walled carbon nanotube buckypaper after acid processing or functionalization. The quality assessment results are consistent with evaluations from the experienced engineers.