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The My Organization tab in ArcGIS Online shows that I've been using lots of credits for Storage.
It's possible that most of this cost is due to a single large dataset that no-one uses, but I can't see any options to sort by size, how frequently the datasets were accessed, etc.
Is it possible to determine which of the many layers in my account are using the most credits?
Clicking on the legend entries will give you a a broad-cut distribution of credit usage, between file storage and data storage, in a table. The table lines are clickable - if detailed info is available, a button to show detailed info will appear under the table as you click on the line. Clicking that button will show your organization detailed credit consumption, by layer, i.e. tagging all layer owners with the credits they use:
