
The Yamaha rider, using both this year's and a prototype of next year's bike, posted a best time of 1:39.429 to outpace yesterday's pace-setter Dani Pedrosa by just 0.018 seconds.
Several riders started their work late before of an overnight rain had left the track wet.
Rossi and Honda's Pedrosa were the only two men who lapped the Spanish circuit in less than 100 seconds, with Jorge Lorenzo already in the 1:40s in the second works Yamaha.
The Honda Gresini team showed promising pace, with Toni Elias in fourth ahead of teammate Alex de Angelis, who completed the top five.
Nicky Hayden was sixth fastest on the only works Ducati on track, although the American finished with the exact same time as de Angelis.
"We've made a big improvement today," said Hayden. "It was important to have back-to-back days with similar conditions because at Valencia we only had one dry day and we weren't able to check that the changes we made to the bike overnight had worked.
"Today my feeling with the bike was much better from the first run and it is important that we've taken over a second and a half off my best time from yesterday.
"We are still a second off the top guys and I know the last second is the most difficult to find but at the same time we're less than a tenth off third fastest and the team is working well, I feel more and more comfortable with the bike and tyres and I can head home with a clear mind. I was pleased that Casey wanted to be here at the test.
"It has been useful to speak with him and Filippo (Preziosi) and it shows how tight the team is and how well everybody wants to do next season."
Mika Kallio was the quickest of the rookies in seventh, while veteran Sete Gibernau was ninth with the new Onde 2000 team.
MotoGP's testing ban kicks off at the start of next month. Pos  Rider             Team                     Time              Laps   1.  Valentino Rossi   Fiat Yamaha Team         1:39.429          54   2.  Dani Pedrosa      Repsol Honda             1:39.447 + 0.018  47   3.  Jorge Lorenzo     Fiat Yamaha Team         1:40.426 + 0.997  58   4.  Toni Elias        San Carlo Honda Gresini  1:40.448 + 1.019  56   5.  Alex De Angelis   San Carlo Honda Gresini  1:40.486 + 1.057  49   6.  Nicky Hayden      Ducati Marlboro Team     1:40.486 + 1.057  70   7.  Mika Kallio       Alice Team               1:40.564 + 1.135  54   8.  Colin Edwards     Tech3 Yamaha             1:40.604 + 1.175  39   9.  Sete Gibernau     ONDE 2000 Ducati         1:40.856 + 1.427  48  10.  Andrea Dovizioso  Repsol Honda             1:40.966 + 1.537  46  11.  Niccolo Canepa    Alice Team               1:41.077 + 1.648  48  12.  James Toseland    Tech3 Yamaha             1:41.740 + 2.311  45  13.  Tonio Guareschi   Ducati Marlboro Team     1:42.906 + 3.477  46  14.  Yuki Takahashi    Scot Racing Team         1:42.918 + 3.489  60 
 
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