In his first innings since March, Pietersen confirmed form and fitness emphatically with a stunning knock that came off 188 balls which included 17 fours and seven sixes.
Pietersen, who has played no cricket since having to leave England's Test tour of New Zealand with bone bruising behind his right knee, was still unbeaten when Surrey declared their first innings close on 353 for seven in response to Yorkshire's 433 for nine.
Yorkshire were 51 for one at stumps in their second innings, a lead of 132.
England managing director Hugh Morris is confident Pietersen will be ready to face Australia in the first Test at Trent Bridge.
Morris told BBC Radio Five's Sportsweek programme: "It's very encouraging that Kevin is back playing again. I know he's worked very hard in practice on preparation and on his fitness. He looks very fit.
"Clearly it's important that he gets some cricket under his belt before the selectors actually sit down and pick the first Ashes squad.
"We've got a few weeks yet and he's got this four-day game and he's in our Twenty20 squad for New Zealand and we've got a game against Essex leading into the Ashes, so there is some cricket left, which is encouraging."
Also in Division One, Derbyshire hold the upper hand in their bottom-of-the-table battle clash with Somerset after day three.
Tony Palladino (five for 97) and Tim Groenewald (five for 30) combined to dismiss Somerset for 216 to earn Derbyshire a first-innings lead of 50 runs, and the home side then reached 36 for two in their second innings before bad light forced the teams off.
At Trent Bridge, Sussex enjoyed a productive second day against Nottinghamshire as they progressed from their overnight first-innings score of 91 for one to 363 for four at the close, captain Ed Joyce (129 not out) and Rory Hamilton-Brown (77no) sharing in an unbroken 158-run stand.