In the early 1900s he toured Australia and New Zealand with Edwin Geach's Popular Dramatic Organisation, and Clarke and Meynell companies.

He then began appearing in movies for Spencer as an actor under the direction of Alfred Rolfe such as Captain Midnight, the Bush King (1911).

Made quickly, with a limited budget and small crew, it was a major financial success and launched his career behind the camera.

He went to work for the Fraser Film Release and Photographic Company for whom he made a feature and a number of shorts, however, they ended the contract after Longford became involved in a lawsuit following the making of the highly popular The Silence of Dean Maitland (1914).

[12] Longford's career revived towards the end of World War I when he helped establish the Southern Cross Feature Film Company in South Australia.

He enjoyed a large box office success with The Woman Suffers (1918) (despite the film being banned in New South Wales) which enabled him to get finance for an adaptation of the poetry of C. J. Dennis, The Sentimental Bloke (1919).

A man coming out of a picture show will be heard to remark to his mate: "s'wonderful the way they get these things up, ain't it, nowadays.'

It was only through the kindness of the American executives in London – the very men against whom I had fought – that I was able to visit studios and get an insight into production conditions.

[26] On his return to Australia, Longford sought financing for a film about the Australian Light Horse in World War I, Desert Legion, with a budget of £50,000.

He managed to direct another feature, The Man They Could Not Hang (1934), although he missed the premiere due to an illness which required hospitalization.

[31] In the same year, he was elected head of the New South Wales Talking Picture Producers Association with the aim of promoting a quota for Australian films.

[37][38] Longford managed to stay employed in the film industry during the 1930s but found this impossible with the advent of World War II, which brought local production to an almost complete halt.

During the war, he was a clerk for the U.S. military stationed in Australia; then he became a tally man and night watchman on the Sydney wharfs.

Longford married Melena Louisa Keen at St Luke's Anglican Church, Concord, Sydney, on 5 February 1900.

Named in Longford and Lottie Lyell's honour, the AACTA Longford Lyell Award is the Australian film industry's highest accolade for an individual based on their contributions to "unwavering commitment over many years to excellence in the film and television industries and has, through their body of work to date, contributed substantially to the enrichment of Australian screen culture".

Since the introduction of the award by the Australian Film Institute in 1968, winners have included Ken G. Hall, Peter Weir, Tim Burstall, Bud Tingwell, David Stratton, George Miller, Phillip Adams, Barry Jones, Jack Thompson, Geoffrey Rush, and Cate Blanchett.