In order to meet high performance liquid crystal displays (LCDSs) demands, fast response display development is an emergency. Motivated by the fact that carbon nanotubes (CNTs) have been proved to improve liquid crystals’ response time effectively and affectively in many ways, doping 3-D single wall carbon nanotube (SWCNT) clusters into alignment layer to decrease electro-optical response time in nematic twist cell has been achieved in this paper. SWCNT clusters existing in SWCNT-Polyimide (PI) nanocomposite were sizes controlled by sonicating and centrifuging SWCNT-PI mixture, and the 3-D structure of these clusters were confirmed by 3-D laser laser beam profiler and Atomic Force Microscope (AFM). The nanocomposite material is directly spin-coated on the indium tin oxide (ITO) glasses, and fabricated into twist nematic (TN) cells after conventional rubbing process. No light leakage had been found in the nanocomposite alignment layer cell, but the voltage to achieve 90% transmittance (V90) of total increases about 41.6% as compared with pure PI alignment layer cell, and the voltage to achieve 10% transmittance (V10) also increased about 17.58%. Superfast switching of the TN LC molecules has been found with approximately an average 10.12% faster in the rising time, an average 29.77% faster in the decaying time and an average 16.12% faster in the total response time in details. The morphology structure change of the alignment layer, electric field enhancement effect from SWCNT clusters and the anchoring strength between LC molecules and SWCNT clusters are the main factors for this super-fast switching of LCs.