We studied the molecular dynamics of chiral and achiral smectic liquid crystals by solid-state ¹³C nuclear magnetic resonance (¹³C-NMR) spectroscopy with a Larmor frequency of 100 MHz. The chiral and achiral smectic liquid crystals used were S-4-(1-methylhexyloxycarbonyl)phenyl 4'-octyloxybiphenyl-4-carboxylate and 4-(hexyloxycarbonyl)phenyl 4'-octyloxybiphenyl-4-carboxylate, respectively. The peak width and the spin-lattice relaxation time were measured to investigate the effect of chirality on the molecular dynamics. The ¹³C-NMR study revealed that introducing chirality, namely, the introduction of a (-CH₃) group to the C23 carbon, affects the intramolecular correlation between the mobility of the carbon and the rotational motion of the aromatic core.