In a previous article [J. Theor. Comput. Chem.2010, 9, 435], all rovibrational bound states of HO2 were systematically computed, for all total angular momentum values J = 0–10. In this article, the high-J rovibrational states are computed for every multiple-of-ten J value up to J = 130, which is the point where the centrifugal barrier obliterates the potential well, and bound states no longer exist. The results are used to assess the importance of Coriolis coupling in this floppy system and to evaluate two different J-shifting schemes. Though not effective for multiply vibrationally excited bound states, vibrational-state-dependent J-shifting obtains modestly accurate predictions for the lowest-lying energies [J. Phys. Chem. A2006, 110, 3246]. However, much better performance is obtained—especially for large J values, and despite substantial Coriolis coupling—using a second, rotational-state-dependent J-shifting scheme [J. Chem. Phys.1998, 108, 5216], for which the rotational constants themselves depend on J and K. The latter formalism also yields important dynamical insight into the structure of the strongly Coriolis-coupled eigenstate wave functions. The calculations were performed using ScalIT, a suite of codes enabling quantum dynamics calculations on massively parallel computing architectures.