We reveal a strongly anisotropic excitonic landscape in monolayer and bulk-like CrSBr using optical absorption spectroscopy and GW-Bethe-Salpeter equation textitab initio calculations. The direct absorptive determination of the lowest bright optical onsets i.e. X₀ᵃ and X₀ᵇ excitons for the two in-plane polarization eigenaxes yield an in-plane optical gap anisotropy of 470 ± 15 meV. This is the highest observed value for any material in the near-infrared-to-visible spectral region to the best of our knowledge. Energetically above, we identify multiple strongly polarized excitons spanning 1.25 eV to 3.1 eV selectively aligned along the two orthogonal axes. A resonance X⁻, located 24 meV below the X₀ᵇ progressively transfers oscillator strength to X_b⁰, a behavior consistent with a coupled trion (Fermi-polarion)/exciton pair. Our experiments also provide polarization-resolved broadband dielectric functions of CrSBr. These results establish CrSBr as a strongly polarization-selective excitonic system and highlight its potential for polarization-selective optoelectronics enabled with its large optical-gap anisotropy.