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World No 7 Casey, who won the Volvo Golf Champions event on the European Tour this season, held a two-stroke lead over fellow-Briton Martin Laird, red-hot Nick Watney and his unheralded compatriots Garrett Willis and Scott Stallings.
Casey, starting at the 10th hole, registered seven birdies without a bogey, capping his stellar card with back-to-back birdies from the seventh at the challenging Copperhead course.
"Today was lovely. Bogey-free is always nice," Casey told reporters after taking advantage of ideal conditions. "It was very benign out there.
"Best ball-striking round of the year. This was fun today," added Casey, who wore a bright green shirt for St Patrick's Day and said precision iron play was the key to his success.
Watney, who won last week's WGC-Cadillac Championship and has finished in the top-10 in each of his five tournaments this year, also got to seven-under with a string of three birdies after making the turn but two late bogeys dropped him to 66.
"I started off great and kind of ran out of steam there at the end," explained Watney, who continued his hot hand with the putter in a round delayed for 70 minutes due to morning fog.
"I putted great last week and the ball, it's just kind of taking off where I'm looking right now which is a really good feeling. Luckily a lot of the putts fell in."
Willis, ranked 277th, had four birdies in a row from the second hole, his 11th hole of the day, to vault into contention. Scotsman Laird posted a bogey-free round, and 25-year-old Stallings had five birdies after making his turn.
Bunched at 67, three shots off the pace, was a group of 10 that included defending champion Jim Furyk, South African Rory Sabbatini and Australians Stuart Appleby and John Senden, who called a one-stroke penalty on himself at the par-five fifth after his ball moved just before he struck his second shot.
Fifteen players were tied another shot back including world No 1 Martin Kaymer of Germany, Fiji's Vijay Singh, Sergio Garcia of Spain and 17-year-old Italian Matteo Manassero.
Kaymer said defending his No 1 status spurred him on.
"Of course I'm thinking about it," US PGA champion Kaymer said. "It's a lot of motivation if you know that you are the best player in the world. So of course I really enjoy that."
Scores on Thursday after darkness halted the first round of the $5.5 million PGA Tour Transitions Championship (USA unless noted, three players yet to finish):
64 - Paul Casey (ENG)
66 - Nick Watney, Garrett Willis, Martin Laird (SCO), Scott Stallings
67 - Joe Durant, John Senden (AUS), Ryan Moore, Gary Woodland, Rory Sabbatini (RSA), Justin Leonard, Webb Simpson, Jim Furyk, Stuart Appleby (AUS), Brian Gay
Notable others:
68 - Martin Kaymer (GER), Marc Leishman (AUS), Sergio Garcia (ESP), Matteo Manassero (ITA), Vijay Singh (FIJ)
69 - Matt Jones (AUS), Arjun Atwal (IND), KJ Choi (KOR), Anders Romero (ARG), Brendon de Jonge (ZIM), Carl Pettersson (SWE), Peter Hanson (SWE)
70 - Charlie Wi (KOR), Geoff Ogilvy (AUS), Jason Day (AUS), Stephen Ames (CAN), Brian Davis (ENG), Justin Rose (ENG)
71 - Ryo Ishikawa (JPN), Nick O'Hern (AUS), Bi-o Kim (KOR), Fabian Gomez (ARG)
72 - Jarrod Lyle (AUS), Stephen Bowditch (AUS), Trevor Immelman (RSA), Retief Goosen (RSA), Nathan Green (AUS)
73 - Padraig Harrington (IRL), Jesper Parnevik (SWE), Alex Cejka (GER)
74 - Greg Chalmers (AUS), Ryuji Imada (JPN)
WD - Richard S. Johnson (SWE) 79
