The total-electron-capture cross section for collisions of C4+ with gr
ound-state hydrogen (deuterium) is measured in the energy range 6-1000
eV/u using the merged-beam technique. The fraction of C4+ metastable
ions present in the ion beam is measured to be 5%, which results in a
correction to the cross section of only a few percent. The independent
ly absolute measurements are generally in good agreement with previous
measurements for total electron capture; however, the reduced uncerta
inties of these measurements allow a more detailed comparison with the
ory. Our observations show that existing fully quantal molecular-orbit
al calculations that include rotational coupling overestimate the cros
s section by approximately 25%. Better agreement is found with a recen
t semiclassical impact-parameter coupled-channel calculation. While al
l available theoretical data predict that the cross section varies smo
othly with energy around the maximum, a sharp structure is observed ar
ound 400 eV/u.