32-bit code can't (directly) call 64-bit code, and vice versa. You have to transition modes, which can really only be done at OS-level. So although I'm not an expert on .Net/C#, I'd say "not possible".
You could build a standalone service process that runs in a 64-bit space and uses the 64-bit DLL, and use interprocess communication to pass data back and forth.
Or compile the DLL as a 32-bit library...