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If your app is compiled targeting x64, you have to use the 64-bit version of the runtime.
If your app is compiled targeting x86, you have to use the 32-bit version.
If your app is compiled targeting AnyCPU, it depends on which O/S your app is running on:
32-bit Windows, must use the 32-bit runtime.
64-bit Windows, must use the 64-bit runtime.