De Villiers was caught by substitute fielder Dimuth Karunaratne off Thisara Perera one short of a 13th test century, but his third straight half-century ensured South Africa was in control of the series opener at stumps on Day 2 at SuperSport Park.
Sri Lanka was bowled out for 180 on Thursday.
De Villiers shared a 97-run partnership for the sixth wicket with Ashwell Prince (39) as South Africa eventually broke free from a stubborn Sri Lankan bowling effort. Perera had 3-114 and took two early wickets as the tourists reduced South Africa to 173-5 before De Villiers and Prince came together.
Brief Scores:
SA: 389 for 9 (de Villiers 99, Smith 61; Thisara Perera 3 for 114) lead SL: 180 by 209 at close of play on Day 2.
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