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He was recalled to the national team in November 2018.

His contract at Ajax was not renewed making him a free agent at the end of June 2017.

On 14 June 2017, fellow Eredivisie club Vitesse announced the signing of Serero on a three-year deal.

In March 2015, he was associated with a move to AC Milan.

On 15 November 2014, Serero scored his first goal for the South African senior team in a 2015 Africa Cup of Nations qualification match against Sudan, scoring in the 37th minute of the 2–1 win at home, thus helping his team secure a berth in the final tournament held in Equatorial Guinea the next year.

On 5 August 2013 he made his debut in the Eerste Divisie, playing for the reserves team Jong Ajax, who had recently been promoted. The match ended in a 2–0 victory against Telstar. On 26 November 2013 he scored his first international goal for Ajax in the UEFA Champions League, when he scored the opener of a 2–1 win at home against FC Barcelona in the 19th minute.

He was released from the national team squad due to disciplinary reasons the day before their 2014 World Cup qualification group match against Botswana on 7 September 2013. According to Gordon Igesund, Serero had allegedly stated to the team doctor that he did not want to play in the match in order to avoid risking an injury ahead of an upcoming UEFA Champions League game for his club. Serero disputed these claims, stating that he was genuinely injured and therefore wary about participating in the game.

During the 2010–11 season, under Foppe de Haan, Serero helped the Cape side to a second place regular season finish scoring 11 league goals, and helped his team to reach the finals of the Telkom Knockout tournament. At the end of the season he was awarded a number of accolades, including PSL Footballer of the Year, PSL Player of the Season, PSL Players' Player of the Season and the ABSA Premiership Red Hot Young Player award. On 22 May 2011, he was signed by AFC Ajax for €2.5 million.

Serero had had several trials with parent club AFC Ajax in the preceding years. On 22 May 2011 it was announced that he had signed a four-year contract with Ajax and he stated it was 'a dream come true'. He made his debut for Ajax on 7 August 2011 coming on as a substitute player in the match against De Graafschap. He only played in a total of 6 matches in his first season with Ajax due to an injury. He scored his first goal for AFC Ajax in the home win against NAC Breda on 25 August 2012. Two weeks later he scored two goals against SC Heerenveen, receiving a red card and being sent off in the same match. On 1 September 2013 Serero made his debut in the starting 11 of Ajax, replacing Christian Eriksen who had just left for Tottenham Hotspur, playing in the midfield.

Serero has played for the South Africa U-20 team. He earned his first cap for South Africa on 9 February 2011. He came on as a second-half substitute in a friendly against Kenya. He scored his first Bafana Bafana goal against Swaziland in a non-friendly match ahead of the 2010 FIFA World Cup.

Born in Mapetla, Soweto, Serero is a product of the Ajax Cape Town's youth academy having been promoted to the first team in 2008, making his debut under then head coach Craig Rosslee. He made a total of 11 appearances in the regular 2008–09 PSL season, and managed to score four times, helping his side to a 7th-place finish by the end of the season. The following season saw Serero become the first choice playmaker at the Cape club, making a total of 25 appearances during the regular season, and scoring twice. Ajax CT would finish in 7th place again that season, with Serero gaining much attention from the local media for his performances on the pitch.

Thulani Caleb Serero (born 11 April 1990) is a South African footballer who plays as a midfielder for Al Jazira and the South African national team. Prior to joining Vitesse , he played for Ajax and for Ajax Cape Town in the South African Premier Soccer League.