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Cambridge is the main city and administrative centre of Cambridgeshire.

In Oxford Advanced Learner’s Dictionary, I think the appropriate definition may be:

  1. belonging to something; being part of something: relating to something example (1): a member of the team

  2. used to say what somebody/something is, consists of, or contains example (2): a city of Dublin

I think the appropriate definition for that sentence should be 2, but example (2) make me feel uncertain.

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    Even the Oxford dictionary couldn't list all the possible meanings of "of". With these kind of small prepositions, I would rely more on understanding how they're used rather than how the dictionary defines them. In this particular sentence the relationship between Cambridge and Cambridgeshire should be obvious.
    – Andrew
    Commented Nov 8, 2018 at 6:29
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    @Andrew is correct. In this case, rather than the example "member of the team" one should think "captain of the team" or "coach of the team." That is, Cambridge fills a role with regard to Cambridgeshire. It is a relationship indicator along the lines of "the A of B."
    – puppetsock
    Commented Nov 12, 2020 at 21:12

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I believe 2. would be correct because the city of Cambridge does not consist of or contain Cambridgeshire. Cambridge is a part of Cambridgeshire.

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