If you mean somehow having PICO-8 itself modify your internet connection, then no (he said confidently, fully expecting a power user to come in and show how it's done).
If you mean having PICO-8 connect to the internet via a different network interface than other applications on your Raspberry Pi, then probably. I haven't ever needed to do this, so I don't know specifically how the routing table configuration would look in this scenario, but you could probably find something in the docs and/or forums for the distro you're using on your Pi.
In general, an app (in userland) should not have the access necessary to change your system settings such as network configuration. This would be a security risk.
I don't have experience with this but couldn't you make an external program that reads the GPIO state from Pico-8 and modifies the internet connection based on that?
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