The ability to control solid-state quantum emitters is fundamental to advancing quantum technologies. The performance of these systems is fundamentally governed by their spin-dependent photodynamics, yet conventional control methods using cavities offer limited access to key nonradiative processes. Here we demonstrate that anisotropic lattice strain serves as a powerful tool for manipulating spin dynamics in solid-state systems. Under high pressure, giant shear strain gradients trigger a complete reversal of the intrinsic spin polarization, redirecting ground-state population from $|0⟩$ to $|\pm 1⟩$ manifold. We show that this reprogramming arises from strain-induced mixing of the NV center’s excited states and dramatic alteration of intersystem crossing, which we quantify through a combination of optomagnetic spectroscopy and a theoretical model that disentangles symmetry-preserving and symmetry-breaking strain contributions. Furthermore, the polarization reversal is spatially mapped with a transition region below 120 nm, illustrating sub-diffraction-limit control. Our Letter establishes strain engineering as a powerful tool for tailoring quantum emitter properties, opening avenues for programmable quantum light sources, high-density spin-based memory, and hybrid quantum photonic devices.

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• Electronic transitions
• Quantum control
• Quantum engineering
• Spontaneous emission