The Si-29 NMR spectra of FAU framework (X and Y) zeolites exhibit a well-resolved splitting into five major bands Si(nAl), where n is the number of first shell aluminum neighbors about silicon. It is well-established that the intensities Si(nAl) reflect the local order resulting from "Al-Al avoidance" in the placement of first-shell (Loewenstein’s rule) and second-shell ("Dempsey’s rule") aluminum neighbors. Study of framework metals ordering in FAU materials has been limited by the information content of the intensities Si(nAl) and by the range of Si/Al compositions available by direct synthesis. Recent synthetic advances have greatly increased the composition range of available materials. In this paper we report Si-29 NMR spectra of 15 directly synthesized FAU zeolites ranging in Si/Al ratios from similar to 1.3 to similar to 5.3. Careful study of the Si-29 NMR spectra reveals considerable information beyond the intensities Si(nAl), manifested in the complex compositional dependence of the band positions and heterogeneous band shapes. The basic premise of this paper is that the Si-29 NMR spectra of FAU zeolites are superpositions of many components arising from the multiple local environments for a silicon atom, these local environments differing in the number and types of first- and second-shell Al substituents. Compositional dependence arises because the relative populations of these local environments are a function of composition. This paper discusses the process by which this additional information has been retrieved and its implications concerning the building units involved in FAU crystallization. The major conclusion is that the immediate precursor to the FAU lattice is the hexagonal prism tertiary building unit and that the secondary unit is the single 4-ring.