Trigonal Na 3 Li(MoO 4 ) 2 ·6H 2 O was found to be an attractive, simultaneously χ (2) -and χ (3) -active nonlinear optical crystal. We investigated its basic optical properties and observed several nonlinear effects, namely many-phonon SRS, almost twooctave Stokes and anti-Stokes lasing combs, SHG, THG, and efficient cascaded (χ (3) ↔ χ (2) )-generation, as well as SRS arising from nonlinear interaction of two different χ (3) -active vibrations. All recorded nonlinear-lasing components were identified and attributed to SRS-promoting vibration modes. A short review of nonlinear-laser molybdates is given.Crystal of Na3Li(MoO4)2·6H2O grown from a seed crystal fixed with its face (001) on a solid base in order to allow only growth along the undisturbed polar direction