Multi-element layered materials enable the use of stoichiometric variation to engineer their optical responses at subwavelength scale. In this regard, naturally occurring van der Waals minerals allow us to harness a wide range of chemical compositions, crystal structures and lattice symmetries for layered materials under atomically thin limit. Recently, one type of naturally occurring sulfide mineral, ternary teallite has attained significant interest in the context of thermoelectric, optoelectronic, and photovoltaic applications, but understanding of light-matter interactions in such ternary teallite crystals is scarcely available. Herein, polarization-dependent linear and nonlinear optical responses in mechanically exfoliated teallite crystals are investigated including anisotropic Raman modes, wavelength-dependent linear dichroism, optical band gap evolution, and anisotropic third-harmonic generation (THG). Furthermore, the third-order nonlinear susceptibility of teallite crystal is estimated using the thickness-dependent THG emission process. We anticipate that our findings will open the avenue to a better understanding of the tailored light-matter interactions in complex multi-element layered materials and their implications in optical sensors, frequency modulators, integrated photonic circuits, and other nonlinear signal processing applications.