Stable lyotropic chiral nematic liquid crystals (N*-LCs) of cellulose nanocrystals (CNs) were prepared via hydrolysis using sulfuric acid. The lyotropic N*-LCs were used as an asymmetric reaction field to synthesize polyaniline (PANI) onto CNs by in situ polymerization. As a primary step, we examined the mesophase transition of the N*-LCs of CNs suspension before and after in situ polymerization of aniline (ANI) by polarizing optical microscopy. The structure of nanocomposites of PANI/CNs was investigated at a microscopic level using Fourier transform infrared spectroscopy and X-ray diffraction. Influence of the CNs-to-ANI ratio on the morphology of the nanocomposites was also investigated at macroscopic level by scanning electron and transmission electron microscopies. It is found that the weight ratio of CNs to aniline in the suspension significantly influenced the size of the PANI particles and interaction between CNs and PANI. Moreover, electrical properties of the obtained PANI/CNs films were studied using standard four-probe technique. It is expected that the lyotropic N*-LCs of CNs might be available for an asymmetric reaction field to produce novel composites of conjugated materials.