The present paper reports the structural and optical properties of PbMo0.75W0.25O4 single crystals grown by Czochralski method. XRD pattern of the crystal indicated well-defined two diffraction peaks associated with tetragonal crystalline structure. Raman and infrared spectra of the grown single crystals were presented to get information about the vibrational characteristics. Observed Raman modes were associated with modes of PbMoO4 and PbWO4. Eight bands were revealed in the infrared spectrum. The bands observed in the spectrum were attributed to multiphonon absorption processes. Transmission spectrum was measured in the 375–700 nm spectral region. The analyses of the spectrum resulted in direct band gap energy of 3.12 ± 0.03 eV. The compositional dependent band gap energy plot was drawn considering the reported band gap energies of PbMoO4, PbWO4 and revealed band gap of PbMo0.75W0.25O4 single crystal. An almost linear behavior of composition-band gap energy was seen for PbMo1-xWxO4 compounds. Urbach energy was also found from the absorption coefficient analysis as 0.082 ± 0.002 eV.