Nuclear polarization plays an essential role in precision measurements, symmetry tests, and emerging quantum technologies, yet efficient polarization of heavy nuclei remains a major challenge. We propose an efficient, intense-laser-based approach that achieves high-efficiency polarization of heavy nuclei through the nonlinear interaction of circularly polarized femtosecond laser pulses with hydrogenlike ions. This scheme enables rapid transfer of angular momentum from light to the nucleus. Numerical simulations show that a single pulse can generate polarization exceeding 10%, while a pulse sequence can drive the system to near-unity polarization. The method is broadly applicable to heavy ions with large hyperfine splittings, as demonstrated for ${}^{229}\mathrm{Th}$, ${}^{205}\mathrm{Pb}$, and ${}^{209}\mathrm{Bi}$. The ability to produce near-complete polarization of large-spin nuclei and heavy ions opens new avenues for nuclear physics and nucleus-based quantum technologies.

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• Fine & hyperfine structure
• Optical pumping
• Photonuclear reactions
• Polarization phenomena