Crystal γ-ray radiation competence on α-quartz crystal up to 15 GPa pressure unveil structural-shielding properties coupling. With increasing pressure the average lattice axial length known as a, and b are decreased affecting the behavior of the observed LAC or HVL values. Via tuning the lattice parameters (4.914<a<4.470 Å) and unit cell volume (113.06<Vc < 89.10 Å3), we were able to optimize the α-quartz crystal shielding performance via adjusting the essential shielding parameters (i.e., (5.809<MAC<0.021 cm2/g), (3.10 × 1023<Neff< 3.74 × 1023 e/g), (10.32<Zeff<12.43), and (10.79<Zeq<11.56)). We find that the maximum value of LAC = 16.61 cm−1 occur at defined unitcell parameters (a = 4.535 Å, c = 5.170 Å c/a = 1.14419, and Vc = 92.09 Å3). Whereas, the LAC minimum value is 12.67246 cm−1 at a = 4.90232 Å, c = 5.38309 Å, c/a = 1.10149, and Vc = 110.91621 Å3). The same is applied on the HVL behavior. This report, confirmed that changing the crystal structural lattice parameters allows for a different chances between the incident radiation-unit cell interactions for a possible optimization against the γ-rays penetrations into the crystal's sub-structures.