We demonstrate that two distinctly different in‐plane epitaxial states ofc‐axis oriented YBa2Cu3O7−&dgr;(YBCO) films on (100) yttria‐stabilized ZrO2(YSZ) single‐crystal substrates can be produced independently, namely, YBCO [100]//YSZ [100] or YBCO [100]//YSZ [110]. Both in‐plane epitaxial relationships can be modeled by matching YBCO and YSZ oxygen sublattices at the film‐substrate interface. High critical current densities (Jc), ∼5×105–1×106A/cm2at 77 K, are achieved when ≳90 vol % of either orientation is present.Jccan be degraded nearly four orders of magnitude in films with mixed orientation.