The abundance of galaxy clusters in the low-redshift universe provides an important cosmological test, constraining a product of the initial amplitude of fluctuations and the amount by which they have grown since early times. The degeneracy of the test with respect to these two factors remains a limitation of abundance studies. Clusters will have different mean assembly times, however, depending on the relative importance of initial fluctuation amplitude and subsequent growth. Thus, structural probes of cluster age such as concentration, shape or substructure may provide a new cosmological test that breaks the main degeneracy in number counts. We review analytic predictions for how mean assembly time should depend on cosmological parameters, and test these predictions using cosmological simulations. Given the overall sensitivity expected, we estimate the cosmological parameter constraints that could be derived from the cluster catalogues of forthcoming surveys such as Euclid, the Nancy Grace Roman Space Telescope, eROSITA, or CMB-S4. We show that by considering the structural properties of their cluster samples, such surveys could easily achieve errors of Δ𝜎 8 = 0.01 or better.