© 2016 American Physical Society. This article reports an improved independent measurement of neutrino mixing angle θ13 at the Daya Bay Reactor Neutrino Experiment. Electron antineutrinos were identified by inverse β-decays with the emitted neutron captured by hydrogen, yielding a data set with principally distinct uncertainties from that with neutrons captured by gadolinium. With the final two of eight antineutrino detectors installed, this study used 621 days of data including the previously reported 217-day data set with six detectors. The dominant statistical uncertainty was reduced by 49%. Intensive studies of the cosmogenic muon-induced Li9 and fast neutron backgrounds and the neutron-capture energy selection efficiency, resulted in a reduction of the systematic uncertainty by 26%. The deficit in the detected number of antineutrinos at the far detectors relative to the expected number based on the near detectors yielded sin22θ13=0.071±0.011 in the three-neutrino-oscillation framework. The combination of this result with the gadolinium-capture result is also reported.