While previous studies have greatly improved our knowledge on the motion capability of the cervical spine, few reported on the kinematics of the entire head-neck complex (C0-T1) during dynamic activities of the head in the upright posture. This study investigated in vivo kinematics of the entire head-neck complex (C0-T1) of eight female asymptomatic subjects during dynamic left-right head axial rotation using a dual fluoroscopic imaging system and 3D-to-2D registration techniques. During one-sided head rotation (i.e., left or right head rotation), the primary rotation of the overall head-neck complex (C0-T1) reached 55.5 ± 10.8°, the upper cervical spine region (C0-2) had a primary axial rotation of 39.7 ± 9.6° (71.3 ± 8.5% of the overall C0-T1 axial rotation), and the lower cervical spine region (C2-T1) had a primary rotation of 10.0 ± 3.7° (18.6 ± 7.2% of the overall C0-T1 axial rotation). Coupled bending rotations occurred in the upper and lower cervical spine regions in similar magnitude but opposite directions (upper: contralateral bending of 18.2 ± 5.9° versus lower: ipsilateral bending of 21.4 ± 5.1°), resulting in a compensatory cervical lateral curvature that balances the head to rotate horizontally. Furthermore, upper cervical segments (C0-1 or C1-2) provided main mobility in different rotational degrees of freedom needed for head axial rotations. Additionally, we quantitatively described both coupled segmental motions (flexion-extension and lateral bending) by correlation with the overall primary axial rotation of the head-neck complex. This investigation offers comprehensive baseline data regarding primary and coupled motions of craniocervical segments during head axial rotation.