The ultrafast nonadibatic relaxation dynamics of the excited state of 2-methylpyrazine has been studied by using femtosecond time-resolved photoelectron imaging and femtosecond time-resolved mass spectrometry. The first excited state S ₁of 2-methylpyrazine was excited by 323 nm pump light, and the excited state deactivation process is detected by 400 nm probe light. The lifetime of S ₁state 98 ps is obtained by time-resolved mass spectroscopy. The intersystem crossing from the S ₁state to the T ₁state is observed on real time. The relaxation dynamics of S ₁state of 2-methlypyrazine is different from that of pyrazine, the results show that the intersystem crossing process between S ₁and T ₁is the main relaxation channel of S ₁state of 2-methlypyrazine, but the internal conversion process between S ₁and S ₀is also a main relaxation channel of S ₁state. By using the advantages of femtosecond time-resolved photoelectron imaging, the photoelectron angular distribution at different pump-probe time delay was obtained experimentally. From the photoelectron angle distribution combined with photoelectron kinetic energy distributions, we tried to observe the field-free nonadiabatic alignment. However, due to the fact that the molecular symmetry of 2-methylpyrazine is lower than that of pyrazine, it is more challenging to observe the phenomenon of molecular nonadiabatic alignment with lower symmetry. Therefore, it is fail to observe nonadiabatic alignment feature of 2-methylpyrazine in this experiment. This work provides a clearer physical picture for S ₁state nonadibatic relaxation dynamics of 2-methylpyrazine.