<p>Nanostructured bismuth (Bi) has become extremely appealing due to its unique optical properties across the UV and near IR spectral regions. It has practical potential in a variety of applications in photonics, including in plasmonics and photocatalysis. This work demonstrates the use of polarization to control the geometry of low spatial frequency (LSFL) laser-induced periodic surface structures (LIPSS) in Bi at a free-space wavelength <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(\varvec{\lambda }_{\varvec{0}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mrow> <mi mathvariant="bold-italic">λ</mi> </mrow> <mrow> <mn mathvariant="bold">0</mn> </mrow> </msub> </math></EquationSource> </InlineEquation> = 1030 nm. This is the first such report for Bi. The symmetry of the periodic nanostructures created is found to be tunable from uniaxial to isotropic by controlling the irradiation polarization from linear to circular. In addition, this work demonstrates the scalability of the polarization-controlled fabrication process in the production of nanostructured areas of mm-squared size on Bi surfaces. Finally, the formation of LSFL is investigated theoretically and numerically using a vectorial model accounting for the coherent interaction of the irradiation field and the multiple scattering of surface plasmon polaritons (SPPs) produced during the LIPSS fabrication process. The model is shown to be in excellent agreement with our experimental observations.</p>