In this study, three-dimensional (3D) nanohybrids with excellent properties were prepared by the simple combination of 1D carbon nanotubes (CNTs) and 2D MgAl-layered double hydroxides (LDHs). An optically active amino acid containing poly(amide-imide) was prepared by direct polycondensation reaction of N-trimellitylimido-l-alanine and 4,4'-diaminodiphenyl methane under green condition in molten tetra-n-butylammonium bromide. PAI/LDH-CNT nanocomposites containing 2, 4, and 8 wt% LDH-CNT were prepared via a simple and an effective ultrasonic method. The presence of CNT in the interlayer space of LDH was confirmed by thermogravimetry analysis, Fourier transformed infrared spectroscopy, and X-ray diffraction techniques. The homogeneous dispersion of nanofillers in the PAI matrix was observed by field emission scanning electron microscopy and transmission electron microscopy. The obtained results revealed the coexistence of exfoliated and intercalated modified LDH-CNT in the polymer matrix.