The spin-pumping mechanism and associated interfacial Gilbert damping are demonstrated in ion-beam sputtered Co2FeAl (CFA)/Mo bilayer thin films employing ferromagnetic resonance spectroscopy. The dependence of the net spin-current transportation on Mo layer thickness, 0 to 10 nm, and the enhancement of the net effective Gilbert damping are reported. The experimental data have been analyzed using spin-pumping theory in terms of spin current pumped through the ferromagnet/nonmagnetic metal interface to deduce the real spin-mixing conductance and the spin-diffusion length, which are estimated to be 1.56(±0.30)×1019m−2 and 2.61(±0.15)nm, respectively. The damping constant is found to be 8.8(±0.2)×10−3 in the Mo(3.5 nm)-capped CFA(8 nm) sample corresponding to an ∼69% enhancement of the original Gilbert damping 5.2(±0.6)×10−3 in the Al-capped CFA thin film. This is further confirmed by inserting the Cu dusting layer which reduces the spin transport across the CFA/Mo interface. The Mo layer thickness-dependent net spin-current density is found to lie in the range of 1−4MAm−2, which also provides additional quantitative evidence of spin pumping in this bilayer thin-film system.