Although epitaxial strain imparted by lattice mismatch between a film and the underlying substrate has led to distinct structures and emergent functionalities, the discrete lattice parameters of limited substrates, combined with strain relaxations driven by film thickness, result in severe obstructions to subtly regulate electro‐elastic coupling properties in perovskite ferroelectric films. Here a practical and universal method to achieve highly strained phases with large tetragonal distortions in Pb‐based ferroelectric films through synergetic effects of moderately (≈1.0%) misfit strains and laser fluences during pulsed laser deposition process is demonstrated. The phase possesses unexpectedly large Poisson's ratio and negative thermal expansion, and concomitant enhancements of spontaneous polarization (≈100 µC cm⁻²) and Curie temperature (≈800 °C), 40% and 75% larger than that of bulk counterparts, respectively. This strategy efficiently circumvents the long‐standing issue of limited numbers of discrete substrates and enables continuous regulations of exploitable lattice states in functional oxide films with tightly elastic coupled performances beyond their present levels.