Organic–inorganic composite films of close-packed, alkanethiol-capped gold nanoparticles and dithiol crosslinkers were assembled at the air–water interface in a Langmuir trough. Mechanical properties were evaluated using Langmuir compression isotherms, providing minimum collapse pressures and qualitative collapse behavior to compare film stability. The data indicate that increased crosslinker rigidity can enhance resistance to collapse relative to flexible linkers, supporting structure–property design criteria for durable nanoparticle films. These results motivate continued measurements to refine component-specific trends and guide the design of nanoarchitectures with targeted chemical, physical, and mechanical properties.