The criticality of ULF (Ultra-low-frequency) magnetic variations is investigated for the 2011 March 11 Tohoku earthquake (EQ) by natural time analysis. For this attempt, some ULF parameters were considered: (1) F h (horizontal magnetic field), (2) F z (vertical magnetic field), and (3) D h (inverse of horizontal magnetic field). The first two parameters refer to the ULF radiation, while the last parameter refers to another ULF effect of ionospheric signature. Nighttime (L.T. = 3 am ± 2 hours) data at Kakioka (KAK) were used, and the power of each quantity at a particular frequency band of 0.03–0.05 Hz was averaged for nighttime hours. The analysis results indicate that F h fulfilled all criticality conditions on March 3–5, 2011, and that the additional parameter, D h reached also a criticality on March 6 or 7. In conclusion, criticality has reached in the pre-EQ fracture region a few days to one week before the main shock of the Tohoku EQ.