The film premiered at the 78th Venice International Film Festival, where it opened to critical acclaim. In 2021, Smit-McPhee starred in Jane Campion's film The Power of the Dog. In 2018, he played the central character Keda, an Ice Age adolescent who tames a wolf, in Alpha. Smit-McPhee reprised the role in Dark Phoenix, which was released in 2019. Smit-McPhee played Nightcrawler in X-Men: Apocalypse (2016), a character whose older version was previously played by Alan Cumming.

Aged 17 when he undertook the role, Smit-McPhee said afterwards that it showed 'that soldiers aren't the patriotic brave souls they look like, it's showing them at their most vulnerable in tragic times and when they are terrified'. He plays 17-year-old Thomas 'Tolly' Johnson, who pretends to be older so that he can enlist with his brother Bevan and ends up fighting at Gallipoli in the campaign that helped create the Anzac legend. In March 2014, he was cast in the Nine Network's seven-part drama series Gallipoli which was broadcast in February and March 2015, the year that marks the 100th anniversary of the Gallipoli landing. Soon afterwards he appeared in Slow West, which was released in 2015. The film premiered at the Sundance Film Festival in January 2014. In 2013, Smit-McPhee filmed the action science fiction film Young Ones. He co-starred in the 20th Century Fox film Dawn of the Planet of the Apes (2014). He also starred in A Birder's Guide to Everything, which premiered at the 2013 Tribeca Film Festival, and played Benvolio in a film adaptation of Romeo and Juliet.

His next role came in The Wilderness of James in the title role of James. Later the same year, Smit-McPhee had a role in Dead Europe, which premiered at the 2012 Toronto International Film Festival. Smit-McPhee then voiced the lead role of Norman in ParaNorman, a 2012 animated comedy horror film which was nominated for Best Animated Feature for the 2013 Academy Awards, and also received a 2013 BAFTA Award nomination for Best Animated Film.

Viggo Mortensen, Smit-McPhee, Joe Penhall, John Hillcoat, and Steve Schwartz at the 2009 premiere of The Road

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