Appearing on the show with her best friend, Abi Finley, Mulholland reached the semi-final, but lost out to Siobhan Dillon in the sing-off in the fifth week, singing "Don't Cry For Me Argentina".

"[9] Shortly after HDYSAPLM finished in December 2006 Mulholland was signed by agents Curtis Brown and promptly took on the part of Roxie Hart, a lead character in the West End musical Chicago.

That December, she was invited back to attend the 10 Year Charity Gala performance and Black Tie Reception to celebrate the production's tenth anniversary.

[13] Although she did not win HDYSAPLM, Mulholland was asked by Andrew Lloyd Webber to take over the role of Maria in The Sound of Music as an 'alternate' on Monday evenings and Wednesday matinees from 16 April 2007, after the winner Connie Fisher had to scale down from eight to six performances a week following medical advice.

[14] In the role of Maria, Mulholland has received strong reviews:[15] Megan Reynolds of The Guardian wrote that her performance was "honest, genuine, heartfelt and passionate, and her songs were pitch-perfect.

On 12 and 13 May 2008, Mulholland appeared at the Royal Albert Hall in Sir Tim Rice's concert revival of his hit musical Chess, with Josh Groban as Anatoly Sergievsky, Idina Menzel as Florence, Adam Pascal as Frederick Trumper, Kerry Ellis as Svetlana and Marti Pellow as the Arbiter.

[20] Mulholland has represented Andrew Lloyd Webber's production The Sound of Music twice at the free event West End Live held in 2007 and 2008.

[21] Between 3 and 5 July 2008, Mulholland starred in her own sold-out show, Sway with Aoife, at the Town Hall Theatre, Galway.

[22] On 18 September 2008 Mulholland starred with the RTÉ Orchestra and Jessie Buckley in Dublin at the Concert Hall, in a Radio Broadcast highlighting songs from the career of Lloyd Webber, who joined her on stage.

[23] At the end of 2008, after leaving The Sound of Music, Mulholland presented a morning report on the Von Trapp family home for BBC Breakfast News.

[citation needed] In November 2008 Mulholland reprised the role of Roxie Hart in Chicago until 12 July 2009, this time starring with both Justin Lee Collins and Jerry Springer.

[citation needed] She was next cast as Brooke Wyndham, in the musical Legally Blonde in London's Savoy Theatre, co-starring with Sheridan Smith, Duncan James and Alex Gaumond.

Whilst training at CSSD, she appeared in many student productions, including Beckett's Play and Come and Go (both directed by Lucy Bailey) as well as The Winter's Tale and The Bright Sun Brings it to Light.