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Johannesburg: The hosts, who began their second innings half-an-hour after lunch, need 454 to win. South Africa won their first Test series in Australia earlier this year, including scoring 414 for four to win the first Test in Perth, the second-biggest successful pursuit in Tests. The record, set by West Indies in 2003, stands at 418.
Smith and fellow opener Neil McKenzie ensured South Africa did not show any early vulnerability as they put on 76 for the first wicket in two hours.
McKenzie was caught behind off Mitchell Johnson for 35 half-an-hour after tea, but Smith batted on for another hour before falling for 69 as he lamely pulled Ben Hilfenhaus to mid-on.
South Africa's resistance continued as Hashim Amla and Jacques Kallis added another 48 runs before the close.
South Africa require another 276 runs in 98 overs on Monday to win the match, but their main priority will be to protect the eight wickets they have in hand on a pitch that is starting to show variations in bounce.
Australia's last pair Peter Siddle and Ben Hilfenhaus had added 33 runs to take their second innings total to 207 after all-rounder Kallis had inspired a South African fightback that brought eight wickets in the morning session as the tourists slumped to 174 for nine at lunch.
Kallis had a capacity crowd buzzing as he claimed three wickets in six balls and took two catches, one an outstanding reflex effort at slip.
Australia found themselves in further trouble on 104 for five in Kallis's next over as Marcus North's innings of five was terminated by a delivery that kept low and bowled him.
Hughes's gutsy 159-minute effort came to an end when he was also outfoxed by Harris, with AB de Villiers taking a brilliant one-handed catch at leg-slip.
Makhaya Ntini then joined the attack to have all-rounder Andrew McDonald, who added just seven to his first-innings duck, and the dangerous Johnson, who scored 96 not out on Friday, caught behind the wicket.
Brief Score: South Africa 220 and 178/2 (Smith 69) required another 276 runs to beat Australia 466 and 207 (Hughes 75)
