The most common and most likely answer to this crossword clue is the 9 letter word CRABBIEST
I've seen this crossword clue in The Guardian
C
R
A
B
B
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Buddy explains!
The straight part
We know that "Most irritable" is the straight/definition part of the clue. The straight part is often a synonym or definition, in this case most irritable = crabbiest.The cryptic/wordplay part
In cryptic crossword there's often an wordplay/cryptic part as well.This part involves a more complex hint, such as an anagram, homophone, hidden word, etc.
Sadly, We don't have an explanation for this specific crossword clue yet.
What does CRABBIEST mean?
CRABBIEST adjective- Visibly irritated or annoyed; grouchy, irritable, in a foul mood; given to complaining or finding fault in an annoyed way.
- Crabbed; difficult, or perplexing.