Metallophthalocyanines (MPcs; M = Zn, Mg) coordinated by 4-amino-TEMPO (ATEMPO) in the excited quartet (Q(1)) state, which are constituted by the excited tripler MPc and doublet ATEMPO, have been studied by a time-resolved electron paramagnetic resonance (TREPR) method. Two components were observed for both the Zn and Mg complexes, and are reasonably assigned to the Q(1) and doublet states by calculating the zero field splitting and g value, respectively. The polarization pattern of the Q(1) ZnPc-ATEMPO is A/E, and is opposite to that (E/A) of the Q(1) MgPc-ATEMPO, where the A and E denote absorption and emission of the microwaves, respectively. The Q(1) TREPR spectrum with the E/A polarization has been observed for the first time. The A/E and E/A polarization patterns are reproduced by selective intersystem crossing (ISC) to \Q(1),+/-1/2'] and to \Q(1),+/-3/2'], respectively. The selective ISC to \Q(1),+/-1/2'] is reasonably explained by the z component of SOC between the Q(1) and higher excited doublet states, while the ISC to \Q(1),+/-3/2'] originates from the x and y components of SOC. These experiments have proved that the selectivity of ISC to the Q(1) state is dependent on the components of SOC.