Nonlinear optical interactions based on χ (2) and χ (3) effects were investigated in the tetragonal, non-centrosymmetric melilite-type crystal Sr2ZnGe2O7. Among them are Stokes and anti-Stokes lasing comb generation, SHG, THG, SFG, and cascaded χ (3) ↔ χ (2) self-frequency conversion, arising from onemicron picosecond pumping. All lasing components were identified and attributed to a single SRS-promoting vibration mode ω SRS ≈ 778 cm −1 . The crystals possess a wide transparency range from ≈ 0.25 μm to ≈ 6.2 μm; their refractive indices show a small birefringence (with an isoindex point at 0.4677 μm wavelength) that does not allow phase matching for χ (2) -based conversion processes.