Raman scattering experiments of natural FeS2 pyrite were performed at simultaneous high-pressure and high-temperature conditions up to 675 K and 2100 MPa using a hydrothermal diamond anvil cell combined with micro-Raman spectroscopy. Four out of five Raman active modes [Eg, Ag, Tg(1) and Tg(3)] were resolved at ambient conditions, the remaining Tg(2) [~377 cm−1] mode was weak and unresolved occurring ~2 cm−1 from the intense Ag [379 cm−1] mode. The frequency shifts of the Eg [343 cm−1] and Ag [379 cm−1] modes were determined to be quadratic functions of pressure and temperature: ν343 = 343.35 – 0.0178 × ΔT – 8.4E–6 × (ΔT)2 + 0.00367 × Δp – 3.7E 7 × (Δp)2 + 1.0E–6 × ΔT × Δp and ν379 = 379.35 – 0.0295 × ΔT – 9.0E–6 × (ΔT)2 + 0.00460 × Δp – 5.3E–7 × (Δp)2 + 7.0E–7 × ΔT × Δp. The positive pressure dependence of both modes indicates stress-induced contraction of S–S and Fe–S bonds, whereas the negative temperature dependence shows temperature-induced expansion of them. The Raman spectra of pyrite were used to derive its bulk modulus at high temperatures, thermal expansion coefficient at high pressures and anharmonic parameters at high-pressure and high-temperature conditions.