During the Expedition Peter Bassett-Smith filmed material used in four coloured cine films directed by Mountford; 'Arnhem Land', a survey of the natural history and ethnology of the region, 'Aborigines of the Sea Coast', showing the life of Aboriginal people at Yirrkala, 'Birds and Billabongs', featuring the birds and water-lilies of Oenpelli Lagoons and 'The Arawaltja Ceremony' of Groote Eylandt.

In his field report to Mountford, Bassett-Smith wrote the following description of filming in Arnhem Land:

'Have you ever tried to weave a small tapestry with fibres from each fleece of Australia's 120 million sheep? No, well try making motion pictures in Arnhem Land. It will be necessary to travel quite such phenomenal distances but 400 miles by [as] planes fly or roughly square miles gives some slight idea of the vast area that has to be covered. There is certainly no lack of material but to present a fair picture on this greatest of Australia's Aboriginal reserves involves transport problems that have to be experienced to be believed; however it is good fun to take shots from the air so we may as well start from there...huddled in the "blister" of a RAAF Catalina, consciousness is rudely thrust upon one with word from the pilot that we are soon to cross the sheer 500 foot sandstone escarpment...with cameras, bristling turret lenses, filters and light meter at the ready, we prepare to go into action. As the silver sky shines up at us from below, reflected in the broad flood plains of the three Alligator rivers that twist like agonised pythons, the sun throws off the mantle of night and we have an unforgettable glimpse. Here is the natural wall of the crowned rocky cliffs and huge rectangular blocks of stone, level strata-ed and solid that, from time immemorial, has guarded the western bounds of this little known country, Arnhem Land. A floating drifting panorama that has gone in an instant. Gone? Well perhaps others may share this vision in the cool dark comfort of an armchair'.