Unilateral vocal fold paralysis (UVFP) causes glottal incompetence and poor vocal efficiency. The influence of laryngeal neuromuscular control on aerodynamics in UVFP remains unclear. This study investigated the relationship between laryngeal muscle activities using quantitative laryngeal electromyography (LEMG) and aerodynamics in UVFP. This prospective study recruited patients with UVFP, and the diagnosis was confirmed with videolaryngostroboscopy and LEMG. The patient received aerodynamic assessment and LEMG of the thyroarytenoid-lateral cricoarytenoid (TA-LCA) muscle complex and the cricothyroid (CT) muscle. The relationship between quantitative LEMG and aerodynamic parameters was analyzed. A total of 134 UVFP patients without concurrent CT muscle involvement were enrolled. Compared with the normal side, the peak turn frequency of the lesioned side was lower in the TA-LCA (p < 0.001) and CT (p = 0.048) muscles. Stepwise linear regression revealed that the turn ratio of TA-LCA muscles was a robust factor in the decrease in peak expiratory airflow (β = −0.34, p = 0.036), mean airflow during voicing (β = −0.28, p = 0.014), and aerodynamic power (β = −0.42, p = 0.019), and an increase in aerodynamic efficiency (β = 27.91, p = 0.012). In addition, the turn ratio of CT muscles was a potent factor in inducing an increase in aerodynamic resistance (β = 14.93, p = 0.029). UVFP without CT involvement still showed suppression of CT muscles on the lesioned side, suggesting that neurological impairment of the TA-LCA complex could cause asymmetrical compensation of CT muscles, further impeding aerodynamics. The residual function of TA-LCA muscle complexes facilitates less air leakage and power dissipation, enhancing aerodynamic efficiency. On the other hand, the symmetrical compensation of the CT muscles improves aerodynamic resistance.