Rolfe acted opposite his wife and father-in-law numerous times around the country throughout the 1890s and early 1900s, most commonly playing juvenile leads.

Among the plays in which Rolfe most frequently appeared opposite his wife and father in law were The Bush King, Robbery Under Arms, and East Lynne.

[9] According to New Zealand's Stage magazine, Rolfe was "an actor of brilliancy on a somewhat wide range, a little overshadowed, perhaps, by the stars with whom he has been so long associated, but by no means obscured.

[17] In early 1909, Rolfe was credited as "general manager" on a series of advertisements throughout New South Wales for a £5,000 film depicting the fight between Tommy Burns and Jack Johnson.

In August 1910 it was announced Rolfe and Lily were joining Philip Lytton's company for a tour of country Australia and New Zealand.

In 1910 Rolfe received an offer to direct three films for Cosens Spencer, all adaptations of productions performed by his father-in-law's and Lytton's company: Captain Midnight, the Bush King, Captain Starlight, or the Gentleman of the Road (an adaptation of Robbery Under Arms), and The Life of Rufus Dawes.

[22] When Rolfe left Spencer, the producer then hired Longford to make his directorial debut with a film adaptation of The Fatal Wedding.

[22] Rolfe ended up making an estimated 25 features for them, including Australia's first war movie (Mates of the Murrumbidgee (1911)), and first film to deal with aboriginal Australians (Moora Neya, or The Message of the Spear (1911)).

[23] After the demise of the Australian Photo-Play Company, Rolfe moved over to Fraser Films, where his movies included adaptations of the popular play The Sunny South (1914) and the poem The Day.

Rolfe said at the same time the greatest difficulty for Australian filmmakers is they are unable to market their films in America or England.

[27] In November 1916 it was announced in the trade press that Rolfe had "severed his connection with Australasian Films after a long period of service.

"[28] Rolfe eventually retired from show business, although he did direct one more film, for charity – the Red Cross sponsored feature Cupid Camouflaged (1918).