What does "I cannot be more thankful" mean?
I want to say that I am very thankful for having this opportunity. Can I say something like the following?
... and I cannot be more thankful for having this opportunity.
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The phrase in the title conveys what it says: an inability to rustle up more thanks. However, the connotation depends on context: words, smile/frown, situation, etc.
It could mean that the little appreciation you’ve expressed is all you can summon, or that you’re so filled with gratitude that you feel like you’d float if you were any more thankful.
In your context, you are expressing sincere gratitude with the phrase, especially if the rest of what you communicate says likewise.