Usually means: Hard candy made from barley.
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We found 19 dictionaries that define the word barley sugar:

General (19 matching dictionaries)
  1. barley sugar: Merriam-Webster
  2. barley sugar: Oxford Learner's Dictionaries
  3. barley sugar: American Heritage Dictionary of the English Language
  4. barley sugar: Collins English Dictionary
  5. barley-sugar: Vocabulary.com
  6. barley-sugar, barley sugar: Wordnik
  7. barley sugar: Cambridge Advanced Learner's Dictionary
  8. barley-sugar, barley sugar: Wiktionary
  9. barley sugar: Infoplease Dictionary
  10. Barley sugar, barley-sugar, barley sugar: Dictionary.com
  11. Barley sugar: Wikipedia, the Free Encyclopedia
  12. barley-sugar: Rhymezone
  13. barley-sugar: Webster's 1828 Dictionary
  14. Barley Sugar: Dictionary of Phrase and Fable (1898)
  15. barley-sugar, barley sugar: FreeDictionary.org
  16. barley-sugar: Mnemonic Dictionary
  17. barley-sugar, barley sugar: TheFreeDictionary.com
  18. barley sugar: Longman Dictionary of Contemporary English

Definitions from Wiktionary (barley sugar)

noun:  A traditional British boiled sweet, yellow or orange in colour, with an extract of barley added as flavouring.
adjective:  Alternative form of barley-sugar [(figurative) Very sweet-natured or saccharine; harmless.]

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