Murnau's Sunrise: A Song of Two Humans and Charlie Chaplin's The Great Dictator and Limelight, he was also one of the cinematographers for the television series Broken Arrow and photographed 19 episodes of My Friend Flicka.

In 1913, Struss, in collaboration with Edward Dickson, Clarence White, Alvin Langdon Coburn, and Paul Anderson, began their own publication, Platinum Print.

In 1914, he resigned his position at the family business and asserted his identity as a professional photographer by assuming Clarence White's former studio space in June of that year [6] At the suggestion of Coburn, Struss submitted prints to the American Invitational Section of the annual exhibition of the Royal Photographic Society in London, initiating an exhibiting practice he would continue into the 1920s.

[8] As Struss continued his exhibitions and specialized commissions, he produced commercial photography for magazines, including Vogue, Vanity Fair, and Harper's Bazaar.

[9] He trained to teach aerial photography, but an investigation into Struss's German affiliations launched by the Military Intelligence Department led to his demotion from the rank of sergeant to private; after a period in confinement in Ithaca, New York, where he had originally gone to teach in the new School of Military Aeronautics, he was transferred to Fort Leavenworth to serve as a prison guard and then as a file clerk.

Near the close of the war, in an attempt to clear his record of rumors of anti-Americanism, he applied and was accepted into Officer's Training Camp at the rank of corporal.

[11] While Struss eventually received an honorable discharge, he likely was disinclined to resume his former roles in New York because of the fracturing of many of his professional relationships in the wake of the military investigation.

[13] In early 1921, he married Ethel Wall, who helped to support him in his photographic work independent of the film studios, which included pictorial views set in California.

Struss's photographic archive of exhibition prints, film stills, negatives, and papers (3 linear feet of materials) is available at the Amon Carter Museum of American Art, located in Fort Worth, Texas.