The Spaniard had struggled with the transition to Bridgestone control tyres for much of the winter before making a breakthrough at the end of the previous test in Qatar.
He then carried that form through to Jerez, beating Rossi to the top spot with a late 1m39.791s lap, 0.070 seconds quicker than the world champion.
With the day starting on a very wet track, Rossi chose to sit out the entire morning waiting for the surface to dry. But once he joined the action he soon established himself at the top of times, where he remained until Lorenzo edged ahead late in the afternoon.
"I am very satisfied because I have improved through every hour of the day today," said Lorenzo. "I was able to confirm the good feeling that I had on the last day in Qatar, when I was second. We still need to keep working, this is just the beginning, but I think we're going in the right way."
Casey Stoner took third for Ducati, 0.115s down on Lorenzo's time, at a track he expects to be his team's weakest.
"Jerez has been our weak point for the last couple of seasons and for some reason our bike just doesn't like it here," he said.
"There used to be a lot of bumps that unsettled it but to be fair a lot of them were ironed out when they relaid the surface and now it's hard to put my finger on the problem. I think every Ducati rider is in the same boat - Jerez is like our kryptonite!"
Suzuki continued their promising winter form, with Chris Vermeulen and Loris Capirossi fourth and sixth. They were split by Colin Edwards, as the Tech 3 Yamaha team made its debut in Monster colours.
Andrea Dovizioso was only seventh on the factory Honda, just ahead of Gresini Honda's Alex de Angelis, who had a fall in the afternoon. Nicky Hayden (Ducati) and Toni Elias (Gresini Honda) completed the top ten.
Marco Melandri had run in the top ten for much of the day on the Hayate Kawasaki, before slipping back to 12th, just behind Tech 3's James Toseland.
On his first appearance deputising for Dani Pedrosa at Honda, former Suzuki rider Kosuke Akiyoshi was 18th quickest.
Tomorrow's test day - the last before the Qatar season-opener - is punctuated by the television 'qualifying simulation' session, in which the fastest rider wins a new BMW road car.
Pos Rider Bike Time 1. Jorge Lorenzo Yamaha 1:39.791 2. Valentino Rossi Yamaha 1:39.861 + 0.070 3. Casey Stoner Ducati 1:39.906 + 0.115 4. Chris Vermeulen Suzuki 1:40.572 + 0.781 5. Colin Edwards Yamaha 1:40.579 + 0.788 6. Loris Capirossi Suzuki 1:40.650 + 0.859 7. Andrea Dovizioso Honda 1:40.821 + 1.030 8. Alex de Angelis Honda 1:40.900 + 1.109 9. Nicky Hayden Ducati 1:40.987 + 1.196 10. Toni Elias Honda 1:41.049 + 1.258 11. James Toseland Yamaha 1:41.122 + 1.331 12. Marco Melandri Kawasaki 1:41.160 + 1.369 13. Randy de Puniet Honda 1:41.168 + 1.377 14. Mika Kallio Ducati 1:41.226 + 1.435 15. Yuki Takahashi Honda 1:41.362 + 1.571 16. Sete Gibernau Ducati 1:41.737 + 1.946 17. Niccolo Canepa Ducati 1:41.851 + 2.060 18. Kosuke Akiyoshi Honda 1:42.286 + 2.495 19. Vittoriano Guareschi Ducati 1:42.324 + 2.533
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