© 2019 American Physical Society. Passivation of barium disilicide (BaSi2) films is very important for their use in solar cell applications. In this paper, we demonstrated the effect of hydrogen (H) passivation on both the photoresponsivity and minority-carrier lifetime of BaSi2 epitaxial films grown by molecular beam epitaxy. First, we examined the growth conditions of a 3-nm-thick hydrogenated amorphous silicon (a-Si) capping layer formed on a 500-nm-thick BaSi2 film and found that an H supply duration (ta-Si:H) of 15 min at a substrate temperature of 180 °C sizably enhanced the photoresponsivity of the BaSi2 film. We next supplied atomic H to BaSi2 epitaxial films at 580 °C and changed supply duration (tBaSi;H) in the range of 1-30 min, followed by capping with an a-Si layer. The photoresponsivity of the films changed considerably depending on tBaSi;H and reached a maximum of 2.5 A/W at a wavelength of 800 nm for the sample passivated for tBaSi;H=15 min under a bias voltage of 0.3 V applied to the front-surface indium-tin-oxide electrode with respect to the back-surface aluminum electrode. This photoresponsivity is approximately one order of magnitude higher than the highest value previously reported for BaSi2. Microwave photoconductivity decay measurements revealed that the minority-carrier lifetime of the BaSi2 film with the highest photoresponsivity was 14 μs, equivalent to its bulk carrier lifetime ever reported. We performed theoretical analyses based on a rate equation including several recombination mechanisms and reproduced the experimentally obtained decay curves. We also calculated the total density of states of BaSi2 by ab initio studies when one Si vacancy existed in a unit cell and one, two, and three H atoms occupied Si vacancy or interstitial sites. A Si vacancy caused a localized state with two energy bands to appear close to the middle of the band gap. In certain cases, H passivation of the Si dangling bonds can markedly decrease trap concentration. From both experimental and theoretical viewpoints, we conclude that an atomic H supply is beneficial for BaSi2 solar cells.