From 2010 until 2012, he led the United Arab Emirates Olympic team in qualifying for the 2012 Summer Olympics in London. It was the nation's very first appearance. On 15 August 2012, he was appointed as UAE's senior national team. He led the country to their third title in 2013 Gulf Cup of Nations. He also led UAE to the third-place finish in 2015 AFC Asian Cup.

Ali took up football with Al Ahli's youth sides at age six, and he progressed steadily through their system. He made his first-team debut at the age of 16 in 1983. Ali won two UAE President's Cup medallions and played a crucial role in the 1988 final against Al Shabab.

Ali was part of the national team for four years, three of them under the Brazilian, Carlos Alberto Parreira, and one year with Parreira's compatriot, Mario Zagallo. The bigger regret he has is not being able to travel to the 1990 FIFA World Cup, the UAE's only appearance in the global event. He himself said: "I was in the 1990 World Cup squad and I was left out because I suffered an injury one week before the team's departure to Italy," he said. "It was a huge disappointment for me."

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