According to Burn, Irrational numbers in English language textbooks, 1890–1915: Constructions and postulates for the completeness of the real numbers, "completeness" was first used by Dedekind in 1872, and then by Hilbert in 1899. This should not be too surprising. Meta-mathematical considerations concerning classes of number systems were rare before axiomatizations, they were studied in concrete realizations, so the term would not have been very useful. Dedekind was a rare exception anticipating later algebraic formalism. Hilbert needed it to distinguish standard geometry from algebraic and non-Archimedean models, and those were not studied until the very end of 19th century.
Both Dedekind's and Hilbert's uses were sporadic, widespread adoption of "completeness" only happened in 1920-s, with the general theory of metric spaces. Dedekind and others did use "continuity" derived from the "continuum" for similar purposes before that. Dedekind seems to prefer "continuity" and talks about "all continuous domains". The least upper bound property and the Archimedean axiom are sometimes called "axioms of continuity" even today.
Here is Burn:
"There is an anachronism in our title, for the widespread use of the term "completeness"
to describe the extension of the rational numbers to the real numbers
only became conventional from its occurrence in the study of metric spaces,
though it was used by Dedekind in [1872] and in his correspondence with Lipschitz
[Dedekind 1876], and by Hilbert in his axioms for geometry [1899] (in every
translation, and every edition after the first).
In the period with which we are
concerned, the issue would generally have been worded differently. How, it
would have been asked, could the continuity of the real line be guaranteed or how
could the continuum be characterized? Dedekind had used the term "completeness"
in [1872] both to describe the closure of a number field under the four
arithmetical operations, and as a synonym for "continuity." We will retain the
modern term ''completeness'' for the sake of clarity, since the term ''continuity,''
in modern usage, applies only to functions."
Dedekind's Stetigkeit und irrationale Zahlen (1872) is translated into English by Berman, it is well-known for developing (Dedekind) cuts. The 1876 letter to Lipschitz is printed in Dedekind's Gesammelte mathematische Werke, vol. 3, p. 473, 1930. Here is from Berman's translation:
"If now, as is our desire, we try to follow up arithmetically all phenomena in
the straight line, the domain of rational numbers is insufficient and it becomes
absolutely necessary that the instrument $R$ constructed by the creation of the
rational numbers be essentially improved by the creation of new numbers such
that the domain of numbers shall gain the same completeness, or as we may say
at once, the same continuity, as the straight line.
[...] The above comparison of the domain $R$ of rational numbers with a straight
line has led to the recognition of the existence of gaps, of a certain incompleteness
or discontinuity of the former, while we ascribe to the straight line
completeness, absence of gaps, or continuity. In what then does this continuity
consist? Everything must depend on the answer to this question, and only
through it shall we obtain a scientific basis for the investigation of all continuous
domains."