Dressed in his trademark Sunday best outfit of red shirt and black pants, he ignited the huge gallery with a two-putt birdie at the par-five first, but that turned out to be his only birdie on the front nine.
He made the turn at eight-under, equal third with fellow Americans Patrick Reed and Sam Burns, and Masters champion Sergio Garcia of Spain. Garcia had only one hole left.
Casey, meanwhile, surged to the front at 10-under after 14 holes as an English one-two finish loomed as a possibility.
Casey charged with seven birdies and one bogey in 14 holes, after starting the day five strokes from the lead.
He led compatriot Justin Rose, who picked up one stroke in eight holes to improve to nine-under.
Casey has won 13 times on the European Tour, but just once on the PGA Tour, at the 2009 Houston Open.
World number five Rose, meanwhile, has been on fire recently with three wins in his past nine starts worldwide.
Overnight leader Corey Conners, meanwhile, came back to earth as the big boys made their moves.
Conners dropped two shots in the first three holes, before settling down to trail by three shots after nine holes.
(Reporting by Andrew Both in Cary, North Carolina, editing by Gene Cherry)
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