As vice-captain

When Sri Lanka toured Bangladesh in February 2006 regular captain Marvan Atapattu was injured and Mahela Jayawardene became captain while Sangakarra was made vice-captain.^[29] Pakistan toured Sri Lanka for two Test and three ODIs in March 2006, and with Atapattu still injured Jayawardene and Sangakkara remained captain and vice-captain respectively.^[30] The pair had only expected to hold the positions on an interim basis, but extended into a third series as Atapattu failed to recover in time tour tour England in April and ended up filling the roles full time.^[31] In July 2006, Sangakkara made his highest Test score to-date (287) against South Africa. In a record-breaking partnership with Mahela Jayawardene, he set up the world record for the highset partnership in Test cricket—624 runs—in this match.^[32]

On 6 December 2007 he made it to the top spot of ICC Test player rankings with a rating of 938, the highest rating ever achieved by a Sri Lankan player, and became the first batsman ever to score in excess of 150 in four consecutive tests.^[13] His skill was recognised worldwide when he earned selection for the ICC World XI One Day International team that competed against Australiain the Johnnie Walker Series in October 2005. Despite the World XI losing all of the one-day games by considerable margins, Sangakkara left the series with some credit, averaging 46. He was one of the winners of the 2008 inaugural Cricinfo awards for outstanding batting in Test cricket.^[33]

Sangakkara holds the record for fastest 8,000 runs (152 innings) in Test cricket. He broke the previous record set by Sachin Tendulkar (154 innings) during the third Test against India on 6 August 2010. He also holds the record for fastest 9,000 runs (172 innings) in Test cricket. He broke the previous record set by Rahul Dravid (176 innings) during the second Test against Pakistan on 3 November 2011.^[34] Sangakkara was billed as a future captain of Sri Lanka.^[35][36] On Sri Lanka's tour to England in May 2006, he was named the vice-captain of the side. On 3 March 2009, aterrorist attack on the Sri Lankan team convoy in Pakistan injured 6 Sri Lankan players including Sangakkara. Sangakkara suffered shrapnel wounds in his shoulder.^[37] In November 2006, Sangakkara made it to the ICC World XI Test team he missed out previous time. Next year, he signed an agreement to join the Warwickshire County Cricket Club.^[38] That year, he scored back-to-back double centuries against Bangladesh and became only the fifth cricketer in the history to do so.^[39]