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This is the normal Sindarin word for “head” (PE17/32, 173; RC/268), which also “often applied to hills or mountains that had not a sharp apex” (PE17/36). Based on the epithet Glórindol “Goldenhead” for Hador (S/147, WJ/234), the word also applied to the head of people (and presumably also animals). In compounds and names it took the form dol, -dol or (mutated) -dhol, as in Dol Guldur, Nardol, or Fanuidhol. Tolkien also represented this word as doll, which is likely its form as an independent word (PE17/32, 36).
Conceptual Development: The earliest precursor to this word was G. nôl “head” in the Gnomish Lexicon of the 1910s (GL/61), cognate of ᴱQ. nóla “head, hill” from the contemporaneous Qenya Lexicon under the early root ᴱ√NOHO “extended” (QL/67). In Early Noldorin Word-lists of the 1920s Tolkien had ᴱN. {naul >>} nod “head” (PE13/150-151), while in The Etymologies of the 1930s he had N. dôl “head” under the root ᴹ√NDOL (Ety/NDOL).
The last of these indicates the noun began with the ancient cluster nd-, which is important because it would affect mutated forms. However, later Sindarin Fanuidhol “Cloudy Head” requires derivation from unstrengthened ✱dol (RGEO/66). In the 1940s, the plural of this word was duil (SM/225; TI/268) which is consistent with a noun ending in a single l (dôl), but Tolkien later represented it as ending in two ll (PE17/32, 36).
Neo-Sindarin: In keeping with Fanuidhol, I think it is best to assume the ancient form of the word began with unstrengthened d-, so that its independent mutated form would be dholl as in ✱i dholl “the head”. As for its plural, it is possible that the cluster ll would resist *i*-intrusion so that the plural form would ✱dyll “heads”; compare gyrth plural of gorth. However, I prefer to assume that final ss, nn, ll clusters were especially weak and still allowed for i-intrusion: compare lais plural of lass and periain plural of perian, versus class-plural periannath. Hence, I would use its 1940s plural form duil, which gives doll “a head”, i dholl “the head”, duil “heads” and i nuil “the heads”.