That’s very far more rare than the TS’s scenario. A test of 100 flips has a SD of 5. So a 67 is 17 above the mean, and that’s 3.4 SD.To answer the TS's question, if you toss a penny 100 times and record your head/tail ratio.
You'll have to do about 1000 sets of 100 tosses to see that 1 to 2 times out of 1000 sets will get a 67/33 distribution or more.