Marc Marquez dipped underneath the outright MotoGP lap record at Jerez to top FP3, while championship leader Andrea Dovizioso and Yamaha's Maverick Vinales missed the Q2 cut.
Cal Crutchlow's 1:38.614s from FP2 stood as the benchmark at the start of the third session, and it only took Marquez nine minutes to better it with a 1:38.549s, while Aleix Espargaro and Mika Kallio jumped up into the Q2 places behind.
Marquez remained unopposed for some time, though Crutchlow reclaimed top spot with a 1:37.973s with half of the session remaining.
However, running the softer rubber for the first time this weekend, Marquez stamped his authority with an unofficial lap record of 1:37.702s on his final lap to go almost three tenths clear of the field.
Crutchlow held onto second on his factory-backed LCR Honda, while Andrea Iannone cemented his place in Q2 with a late effort of 1:37.989s to jump up from outside of the top 10.
Johann Zarco was top Yamaha runner again at Jerez on his Tech3 M1, the French rider four tenths off the pace with a 1:38.163s, with Ducati's Jorge Lorenzo 0.022 seconds behind to complete the top five.
Pramac's Jack Miller was a further 0.039s adrift, while seventh-placed Valentino Rossi is so far the only factory Yamaha rider contesting the second part of qualifying, after teammate Maverick Vinales could only manage 12th in the frantic final minutes of FP3.
Dani Pedrosa, on the second Repsol Honda, the sister Pramac bike of Danilo Petrucci and Suzuki's Alex Rins secured the final Q2 places, with Dovizioso missing out on his final run by just 0.043s.
Aprilia's Espargaro had sat inside the Q2 places for much of the 45 minutes, but was shuffled back to 13th at the chequered flag ahead of Tito Rabat, who was also set for a place in Q2 before a late fall at the Pons corner.
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