In the first Test against Pakistan in 2015, Ali struggled with the ball, conceding 121 runs in the first innings without taking a wicket, although he did take two wickets in the second innings. In his new role as opener, he made 35 with the bat in the first innings and 11 in the second as the match ended in a draw. In the first innings of the second Test, he took figures of 3–108, but again struggled with the bat, making scores of 1 in both innings as England slumped to defeat. He took 2–49 in Pakistan's first innings as they were dismissed for 234 in the third Test, although he only scored 36 runs in the match as England lost by 127 runs.
Ali is an Ambassador of StreetChance, a programme providing free weekly cricket coaching sessions in deprived areas in the UK, run by the Cricket Foundation and Barclays Spaces For Sports. In January 2015, he joined Orphans in Need, an international NGO, as a Global Brand Ambassador and carried the charity's logo on his bat. Speaking after his stint at the crease, Moeen Ali said, “I enjoy coming back to the community where I grew up playing tapeball cricket. It keeps you grounded. I hope that, as an ambassador for the charity, I can pass on some useful advice and help inspire children like the ones here today involved in StreetChance. It’s so important that schemes like StreetChance give young people the opportunity to play cricket and to learn key life skills, wherever they’re from, whatever their background.”
In January 2015, Ali was nominated for the Best at Sport award at the British Muslim Awards.