The Raspberry Pi doesn't have enough pins, nor the speed to react to those pins, to replace an m68000 processor. You'll just have to wait for the Vampire 500 for that.
On the other hand, there's no good reason a Raspberry Pi couldn't be used to provide an older Amiga with ethernet and storage, and perhaps some other services. With 17 or so GPIO, it wouldn't be ideal to use a Pi as a Zorro expansion because it'd take a bit of circuitry to multiplex the address and data busses for the GPIO, but it's possible.
What's within the realm of possibility with just a handful of wires is a parallel port to Raspberry Pi connection for ethernet and storage. One would just have to adapt some of the drivers which already exist in Aminet to the Pi.
I've used Pis and other small computers (PogoPlugs, Beaglebones) to speed up compiling on retrocomputers. Right now a faster machine is helping my m68060 Amiga 1200 compile binary packages for NetBSD. If we had newer toolchain tools for AmigaDOS, some of this might be applicable.
https://hackaday.io/project/218-speed-up-pkgsrc-on-retrocomputers