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Would it be faster to connect through USB? I would think that it would...
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Unfortunately CC can't be used via USB. What you want to do is possible. In fact, I've done myself several times in the last nine years. You just skipped an important step.
As chaley indicated above you need to duplicate the library on the first device. Doing this is a three-step process. First, backup the library on the first device. Second, copy the backup file and the entire directory structure to the second device and restore the backup from the first device on the second. Third, in CC go to Settings > Formats and folders and change the location, if necessary, to the new location.
If the library is on an external SD and even if the directory structure is the same, you will still have to reselect the directory on the card since the UUIDs of the two cards will be different and will appear as something like storage/NNNN-NNNN/Books with NNNN-NNNN being the specific UUID of each SD Card.
Then you can sync both libraries to the same source Calibre library.