The present work gives a brief review of the nonlinear χ(2)‐ and χ(3)‐lasing properties of SRS‐active natural crystals (minerals) known so far. This compilation complements new results of a detailed investigation of Raman induced χ(3)‐effects in aragonite single crystals (orthorhombic CaCO3) under single‐ and dual‐wavelength picosecond excitation in the UV, visible and near‐IR spectral ranges. The studied effects at room and cryogenic temperatures comprise Stokes and anti‐Stokes combs of almost two octaves bandwidth, THG, SFG, as well as cascaded and cross‐cascaded χ(3) ↔ χ(3) interactions. All recorded lasing χ(3)‐components were identified and attributed to three observed SRS‐promoting vibration modes ωSRS 1 ≈ 1087 cm–1, ωSRS 2 ≈ 152 cm–1, and ωSRS 3 ≈ 205 cm–1 (at room temperature) of aragonite. Stimulated Raman scattering (SRS) investigations of minerals so far enrich the arsenal of SRS‐active crystals, which can be applied to solve fundamental and applied tasks of modern laser physics and nonlinear optics. (© 2012 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA) (© 2011 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA)