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Understanding the nature of the luminous 1991T-like supernovae (SNe) is of great importance to SN cosmology as they are likely to have been more common in the early Universe. In this paper, we explore the observational properties of 1991T-like SNe to study their relationship to other luminous, slow-declining Type Ia supernovae (SNe Ia). From the spectroscopic and photometric criteria defined in Phillips et al., we identify 17 1991T-like SNe from the literature. Combining these objects with 10 1991T-like SNe from the Carnegie Supernova Project-II, the spectra, light curves, and colors of these events, along with their host galaxy properties, are examined in detail. We conclude that 1991T-like SNe are closely related in essentially all of their UV, optical, and near-infrared properties—as well as their host galaxy parameters—to the slow-declining subset of Branch core-normal SNe and to the intermediate 1999aa-like events, forming a continuum of luminous SNe Ia. The overriding difference between these three subgroups appears to be the extent to which ^56 Ni mixes into the ejecta, producing the premaximum spectra dominated by Fe iii absorption, the broader UV light curves, and the higher luminosities that characterize the 1991T-like events. Nevertheless, the association of 1991T-like SNe with the rare Type Ia circumstellar material SNe would seem to run counter to this hypothesis, in which case 1991T-like events may form a separate subclass of SNe Ia, possibly arising from single-degenerate progenitor systems.