Ty setting the build action on the item to 'Content'. Set the 'Copy to output directory' setting to 'Copy always'. Make sure you add the native DLL to your test project, as this is the one that will be primarily hosted in the runtime environment. You can inspect the contents of the workspace by right-clicking on the failed build in the Tests Window an examining it in windows explorer. If things are configured right, MSBuild should treat the unmanaged DLL as a resource that is always copied adjacent to the test DLL when it builds the project. In this way, it sits in a resolution path for the code when the tests run.
You can find more information about
NCrunch workspaces here.
Another option is to manually load the DLL inside your test code prior to it being needed, using Assembly.LoadFrom and specifying a path to the DLL. This is a bit messier as you need to be sure the code will always run before the DLL is needed (a SetUpFixture or equivalent might be the best option for this).