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The 26-year-old Steyn returned with a career-best haul of seven for 51 as the hosts were bundled out for 233 in the first innings and suffered the ignominy of follow-on despite Virender Sehwag's aggressive 109.
Trailing by a mammoth 325 runs, the Indians were struggling at 66 for two in their second innings at close of play on an eventful third day's play which saw the hosts lose as many as six wickets in the span of 12 runs immediately after the tea break.
Murali Vijay (27) and Sachin Tendulkar (15) were at the crease at stumps with India still needing 259 runs to make the visitors bat again.
The Indians were cruising along at 221 for four at the tea interval but the complexion of the game changed in a matter of few minutes with Mahendra Singh Dhoni (6) and debutant S Badrinath (56) departing in quick succession. The tailenders also caved in without much resistance.
Resuming at 25 for no loss, the Indians lost Gautam Gambhir (12), Murali Vijay (4) and Sachin Tendulkar (7) in the pre-lunch session but Sehwag and Badrinath steadied the ship to some extent.
But Sehwag's dismissal just before the tea break opened up the floodgates with Steyn virtually ripping through the lower order in a dramatic spell of seam bowling.
With two full days left, the Indians now have the daunting task to save the game but it looks a tall order with seasoned batsmen like Rahul Dravid, VVS Laxman and Yuvraj Singh not playing the match because of injuries.
A defeat will make it difficult for India to retain its number one status in Test cricket as they would have no other option but to win the next game in Kolkata to stay at the top. South Africa need to win the series by 1-0 margin to dethrone India from the top position.
Earlier this morning, the pace duo of Steyn and Morne Morkel dished out fiery spells to dismiss Gambhir, Vijay and Tendulkar cheaply before the home team recovered through the enterprise shown by Sehwag.
The first to go was Gambhir without adding a run to his overnight score of 12. He was out to the first ball he faced from the tall Morkel, edging it to wicketkeeper Mark Boucher.
Vijay, playing in only his fourth Test match, made a grave error in judging a delivery from Steyn that swung and crashed into the stumps.
Worse was to follow as Steyn brought Tendulkar forward for a drive with a late out-swinger that the ace batsman could only edge to Boucher.
Sehwag cracked a fluent 109 off 139 balls to lead the home team's fight-back along with Badrinath, who hit a half-century in his maiden innings, before slashing a wide Wayne Parnell delivery to give a straight-forward catch to JP Duminy in the deep.
The four-wicket partnership had yielded 136 runs in 197 balls and lifted India from a precarious 56 for three to 192 for four.
Once Sehwag departed, Steyn triggered a batting collapse with his 13th five-for and the hosts eventually folded inside 65 overs.
India's second innings was hardly any better with both the openers, Gambhir (1) and Sehwag (16), returning back in the dressing room inside five overs.
Morne Morkel brought one back from outside the off-stump and a shoulder-arming Gambhir watched in horror as the ball pegged back his stump.
Sehwag was not at his best either, receiving a Morkel delivery on his rib cage that required medical attention.
In the next over, Sehwag tried to slash a Steyn delivery but managed just an edge which flew into Graeme Smith's palm in the first slip as India slumped to 24 for two.
Tendulkar and Vijay maintained a strict vigil to ensure there was no further setback in their second innings.