The spectral dependences of transmission and absorption in the wavelength range of 200–2500 nm were measured for Ca3TaGa3Si2O14 crystals cut perpendicular to the optical axis in the initial state (without annealing) and after isothermal annealing in vacuum and in air. It was found that annealing in vacuum leads to a decrease, and annealing in air leads to an increase in the intensity of absorption bands. A spectrophotometric method for measuring and calculating the specific rotation angle ρ of the plane of polarization of light in gyrotropic crystals from the transmission coefficient spectra at different angles between the polarizer and the analyzer is considered. The transmission spectra were normalized in order to eliminate shifts in the spectra associated with measurement features. Spectral dependences of the values of ρ for all three samples, which are approximated by the extended Drude formula, are obtained; the influence of the annealing atmosphere on the values of the coefficients of this formula is established.