Scorecard
South Africa, who made a mamoth 517 in their first innings, removed both Pakistan openers, Shan Masood and Khurram Manzoor, without scoring before lunch to further close in on a series-levelling win at Dubai stadium.
Pakistan also lost Azhar Ali (19) and were strugglng at 56 for three at tea with Younis Khan (29) and skipper Misbah-ul Haq (seven) at the crease.
They need another 362 runs to avoid an innings defeat. Dale Steyn gave South Africa an ideal start as he removed Masood with the fourth ball of the innings, having him trapped in front of the wicket with a sharp delivery, much to the dismay of Pakistan who needed a good start.
It became two for two when Manzoor fell for his second duck of the match, caught off a miscued drive off Vernon Philander from the fifth ball of the second over.
Manzoor had made 146 in Pakistan's seven-wicket in last week's Abu Dhabi Test.
Azhar Ali and Younis added 46 for the third wicket before part-time spinner Jean-Paul Duminy struck with his first ball, trapping Ali lbw with a low delivery.
Duminy could have taken Younis on 28 but Kallis failed to hold a low catch in the slips.
Pakistan were bowled out for a paltry 99. In the morning session, South Africa lost their last six wickets for the addition of 57 runs after resuming at 460-4. Off-spinner Saeed Ajmal finished with 5-161 while paceman Mohammad Irfan took 3-102.
De Villiers (164) was the first man to go, caught behind off Irfan in the fifth over of the day.
He hit 17 fours and a six during a commanding 376-minute innings and completed an all-time South African fifth wicket record partnership of 338 with Smith.
Irfan could have removed Smith in his next over but Akmal once again faltered behind the stumps, dropping a shoulder-high catch to his left.
But unlike Akmal's dropped catch, when De Villiers had a let-off on the very first ball on Thursday, this didn't prove costly as Smith was caught in the slip by Younis Khan in Saeed Ajmal's next over.
Smith's superb knock lasted 10 hours and 32 minutes during which he dominated Pakistan's bowling, hitting 16 fours and faced 388 balls.
With Smith's catch, Younis beat Javed Miandad's record of most Test catches of 93. It took him 86 Tests, 38 fewer than his illustrious countryman.
Irfan removed Duminy for seven before he was forced out of attack by Australian umpire Rod Tucker for running into the danger zone after a second warning.
Ajmal then wrapped up the innings with the last three wickets to complete his ninth five-wicket haul in Tests.
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