It depends on the code that generates or uses the cache entries, but they're supposed to be OK to delete; applications shouldn't rely on the cache as a permanent data store.
Usually, caches are a result of doing something that takes time to do (so you don't have to do it every time you need the same result). If you delete the cache files, those tasks will need to run fully, and are likely to generate new cache files at the time (if the cache library is turned on).
If those functions that take time to run no longer work properly, or called out to external services that are no longer active or available, then some things might not work.
Your safest option would be to find all instances in the code that uses the cache, and determine if it's safe to delete the files that match that usage.
The quickest option would be to delete the cache files and hope for the best.
Whatever you delete, it's recommended to keep the index.html and .htaccess files.