Is there any way to increase the capacity of these?
Are there any upgrades available for the 3rd Gen iPod shuffle to go to 8GB or more?
no, there is no upgrade possibility.
as you dan see in the shuffle teardown/step 13:
The primary (and only) chip, which is a multi-layered stack containing the CPU, RAM, and 4GB of flash memory.
so there is no "simple" flash memory in the shuffle and that fact makes an upgrade impossible
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