A colorless Ce3+-activated borosilicate scintillating glass enriched with Gd2O3 is successfully synthesized in air atmosphere for the first time. The full replacement of 10mol% BaO by Al2O3, and the partial substitution of 3mol% SiO2 by Si3N4 in the designed glass composition are crucial for this success. The role of Al3+ on tuning the optical properties of Ce3+-activated borosilicate scintillating glass synthesized in air are analyzed by optical transmittance, X-ray absorption near edge spectroscopy (XANES) spectra, photoluminescence (PL) and radioluminescence (RL) spectra. The results suggest that the stable Ce4+ ions can be effectively reduced to stable Ce3+ ions by the full replacement of BaO by Al2O3, and both the PL andRL intensity of the designed borosilicate scintillating glass are enhanced by a factor of 6.7 and 5.2, respectively. The integral RL intensity of the synthesized Ce3+-activated borosilicate scintillating glass is 17.2%BGO, with a light output of about 1180ph/MeV. The strategy of substituting BaO by Al2O3 will trigger more scientific and technological considerations in designing novel fast scintillating glasses.