[citation needed] Her first lead role was playing Polly Peachum in Jonathan Miller's production of The Beggar's Opera at Wilton's Music Hall in London.

[citation needed] In 2018, McGregor developed the operatic cabaret Lorelei based on the myth of the sirens on a rock above the Rhine who lured sailors to their death.

Her solo shows Midnight Lullabies and Evergreens also debuted at The Famous Spiegeltent as well as playing at The Butterfly Club in Melbourne and at Adelaide and Edinburgh Fringe Festivals.

[citation needed] Her variety show Ali McGregor's Late-Nite Variety-Nite Night has become a fixture at The Melbourne International Comedy Festival;[4] guests include Hamish & Andy, Danny Bhoy, Tim Minchin, Eddie Perfect, Julia Zemiro and Rima the Itty-bitty Belly-dancer.

As an actress, McGregor has appeared in various TV commercials in the UK for companies including Norwich Union, BBC, Eircell, Pontiac Grand Prix, Bliss Jewellery and BN Biscuits.

McGregor was an occasional guest panellist on the ABC music quiz show Spicks and Specks which was hosted by her husband Adam Hills.