At this time, GPU.NET only supports nVidia-based devices which are "CUDA-capable". You can find a list of these devices on nVidia's CUDA website.
NOTE: We recommend updating any machines using GPU.NET to the most recent drivers available for your hardware. As of v2.0.0, GPU.NET requires a minimum CUDA version of 4.0.
GPU.NET supports 32- and 64-bit versions of Microsoft Windows XP/Vista/7 and Windows Server 2008/2008R2.
Linux and Mac OS X will be supported via Mono in an upcoming release. (Est. Q2 2012)
The GPU.NET Toolkit, Runtime and vendor-based Plugins are compatible with the 2.0 (and newer) versions of the .NET Framework.