Depending on the system, the characteristic length, or period, of these patterns can vary from a few nanometers (as in directed self-assembly of block copolymers in nanolithography) [4] to a few microns (as in ripple patterns of alternating superconducting and normal regions in type-I superconductors) [7] to centimeters (as in convective roll patterns in CO 2 gas undergoing a Rayleigh-Benard instability). [8] It is the presence of multiple competing interaction forces that gives rise to such spatial inhomogeneities in otherwise uniform ground states. Such modulations can also arise in other order parameters, such as magnetization in films of rare-earth garnets and polarization in ferroelectric films. For example, in thin plates of barium scandium ferrite, application of a magnetic field has been shown to transform the stripe domain state into a periodic array of magnetic bubbles/skyrmions due to the interaction between the long-range magnetodipolar force, Dzyaloshinskii-Moriya interaction, and exchange interactions. [9] Ferroelectric materials also provide a rich design space for tuning material structure and properties by changing mechanical and electrical boundary conditions. For example, interesting modulations of polarization including polarization vortices, [10] skyrmions, [11] and merons [12] can be observed as one manipulates the energy balance with the boundary conditions. More generally, when grown as films on an appropriate crystalline substrate, ferroelectric materials can accommodate lattice-mismatch stress by forming various patterns of ferroelastic domains. [13] In the case of a tetragonal ferroelectric such as PbTiO 3 grown on REScO 3 substrates (where RE = Dy, Gd, Tb, Sc, Nd), [14] different types of 90° domain configurations form, either so-called c/a (wherein the polar axis alternates from being aligned along the out-of-plane and in-plane directions from domain to domain) or a 1 /a 2 (wherein the polar axis is always aligned in the plane of the film, but alternates between being aligned along the [100] or [010]) domains can be achieved depending on the strain imposed by the substrate. [15] Furthermore, these domain structures, when controlled to have similar energies, can produce coexisting mixed-phase polarization structures. [16] Such coexisting structures have been shown to exhibit facile interconversion between polarization states upon application of mechanical [17] and electrical [18] stimuli.The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice-mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain-driven control of hierarchical domain structures in Pb 1−x Sr x TiO 3 solid-solution thin films wherein two types, c/a and a 1 /a 2 , of nanodomains can coexist. Combining phase-field simulations, epitaxial thin-film growth, ...