We report an effective substitution of aluminum for gallium in langasite-type La3Ta0.5Ga5.5O14 (LTG) crystals for use in a pressure sensor at high temperature. Al-substituted LTG (La3Ta0.5Ga5.5-xAlxO14; LTGAx) single crystals up to the solubility limit of x=0.5 have been grown by the conventional Czochralski technique. The electric properties of the LTGAx crystals were investigated and compared with those of LTG. By Al substitution, the piezoelectric constant d11 and the electromechanical coupling factors (k12) became slightly larger. The LTGAx crystals showed a lower temperature dependence of d11 and a higher electric resistivity ρ than those of the LTG crystals.