Alliterate is the act of using alliteration which is the repetition of initial consonants in the beginning of two or more words immediately succeeding each other or at short intervals.
"The poem would look much nicer if you could alliterate the first few lines."
Illiterate is the act of being unable to read or write - having less than expected standard of familiarity with language and literature or education in general.
"Most of the manual labourers are illiterates."
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