Stokes' flawless 112, which included three successive sixes in the course of bringing up three figures, helped the hosts to 353 all out.
Roland-Jones then ripped through the South Africa top order as the Proteas slumped to 61-7 before closing on 126-8, still 28 runs shy of the follow-on target.
Though the weather forecast is mixed for the weekend, Joe Root's men look set to take a 2-1 lead in the four-match series.
That would represent another familiar swing in the fortunes of the England side, who won handsomely at Lord's only to be annihilated at Trent Bridge.
South Africa was hampered by the absence of Vernon Philander, the pace bowler sent to the hospital after a stomach complaint worsened, while their batting was decimated in ideal conditions for pace bowling.
Philander will spend Friday night on a drip and is unlikely to play any part on Saturday.
- Roland-Jones' dream day, and why Trueman would approve - Agnew
- How the South Africa collapse happened - analysis & highlights
Who is England's new hero, Toby Roland-Jones?
Fast bowler Roland-Jones, 29, made his one-day international debut in May and got the chance for a first Test cap after an injury to Mark Wood.
A batsman as a youngster at Middlesex, he was persuaded to take bowling more seriously by former England international Angus Fraser and sealed last season's County Championship with a hat-trick against Yorkshire.
Tall, broad and with a long, languid approach, he exploited the dark, damp conditions by moving the ball in the air and occasionally extracting spitting bounce at speeds of just over 80mph.
Dean Elgar was caught behind, Heino Kuhn trapped lbw playing across the line and Hashim Amla gloved a brutal delivery that reared towards his throat.
When Quinton de Kock was caught at gully off a leading edge, Roland-Jones had taken 4-15 in 24 balls.
James Anderson then got in on the act, with Faf du Plessis lbw offering no stroke and Chris Morris, who earlier struggled with the ball, caught and bowled.
Stokes had a wafting Keshav Maharaj caught at first slip as South Africa faced the indignity of following-on before the close.
Temba Bavuma could have been given out caught off an inside edge from his first ball, delivered by Roland-Jones, but added 53 with Kagiso Rabada.
With Philander absent, England had about six minutes to take the ninth and final wicket, but Morne Morkel accompanied Bavuma to the close.
Thrilling Stokes rewarded for hard work
Stokes had laid the foundations for his second-day brilliance with the hard work he did on the first evening in testing circumstances.
With England resuming on 171-4, they lost former captain Alastair Cook lbw to Morkel for 88.
Philander managed only five overs and, when South Africa turned to their change bowling, Stokes tucked in with drives and pulls.
Jonny Bairstow impressed for 36, Roland-Jones hit four fours and a six in his 25-ball stay and, overall, England showed all the care, application and determination that was lacking at Trent Bridge.
Stokes was on 91 when the ninth wicket fell, Anderson surviving three deliveries before the thrilling entertainment began.
Stokes attacked spinner Maharaj with blows over the leg side - the first was carried on to the rope by Du Plessis, the second brought up his century and the third made him only the second England player to hit three successive maximums in a Test.
Stokes was the last man out, caught at long-off looking to launch Morkel, but only after he had delighted a noisy Oval and taken England to a strong total.
'Stokes knock one of the best' - TMS analysis
Ex-South Africa skipper Graeme Smith: "Ben Stokes' innings was one of the best innings you'll see. He showed poise and determination on the first day, and he's got his side into a really good position today."
Former England captain Michael Vaughan: "Stokes has played some real quality innings but I don't remember seeing him batting in such a mature way, to leave so many balls and wait for a straight one or a short one.
"It was full of determination and the way England batted in the first innings is exactly the way I expect to see them bat on a regular basis."
Debutant TRJ's 'special' day
England's Toby Roland-Jones told BBC Sport: "It was a pretty special day, we wanted to push ourselves as high as possible in some testing conditions.
"There were still some nerves at the top of the mark, but it always helps when you've got guys like Jimmy [Anderson] and Stuart [Broad] who guided me through the opening few overs, and I was on adrenaline after that.
"Particularly in the context of the game, we stand here on day two in a pretty strong position. The Amla wicket was probably the best of the bunch, with all that he's done in the game."
England's new boy's instant impact - stats corner
- Roland-Jones took 5.3 overs to get to four Test wickets, the second fastest for England. Bob Appleyard is the fastest, in 4.3 overs, against Pakistan at Trent Bridge in 1954.
- If Roland-Jones takes one more wicket in South Africa's first innings he will be the first player since Graham Onions in 2009 to take 5+ wickets in their debut bowling innings for England.
- George Simpson-Hayward is the last double-barreled England bowler to take five wickets in an innings.
- Ben Stokes is only the second Englishman to hit three consecutive sixes in a Test match. The only previous player to do so was Wally Hammond, hitting Jack Newman for three sixes at Auckland when he made 336 not out.
What you said - Twitter reaction
- Critchley: There's something very Angus Fraser about TRJ... a bit handier with the bat mind.
- Roy Cole: Toby Roland-Jones = Glenn McGrath
- Barney: Ben Stokes will never have the career stats of South African great Jacques Kallis but I'd suggest he will win more games than Kallis throughout his career.
- James Matthews: Comparison to Kallis silly, but Stokes already has a same number of five-fors and 100s as Andrew Flintoff.
- Jack Taggart: Importance of Cook's innings can't be underestimated. Got them through a tough time and allowed Stokes to show his true class.
And finally... will England enforce the follow-on?
Ex-England captain Vaughan, talking on Test Match Special, thinks not.
He said: "I would doubt Joe Root will enforce the follow-on tomorrow now, but if he had got half-an-hour at them this evening I think he would have done."
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