An experimental study has been performed to demonstrate the advantage of employing ambient helium gas in the spectral quality improvement of hydrogen emission in laser-induced plasma from zircaloy-2 samples at both atmospheric and low gas pressure. It was further shown that the optimal results achieved in the two pressure regimes require the adoption of different sets of experimental parameters consisting of the laser energy, the focusing lens position and the detection gate delay. A strictly linear calibration line with extrapolated zero intercept was nevertheless exhibited in the case of atmospheric gas pressure only. Additional time-evolution measurement of the emission intensities of hydrogen, helium and zirconium clearly suggests a distinctly different excitation mechanism for hydrogen atoms associated with the presence of ambient helium atoms and their meta-stable excited state.