It is possible, to an extent. You can't do it with an MSI alone, though. An example of this is Microsoft's .NET installer packages; the "full install" package has x86 bit, x64 bit, and ia64 support. However, this installer uses a bootstrapping process to do it; it has a separate program that determines exactly what to install, and then installs it. Underneath, you still need the 32 bit MSI and the 64 bit MSI packages.
Be warned though; the architecture of your installer's bootstrapper will then determine what it can be installed on. If it's an x86 based bootstrapper, then it will only work on 32 bit windows and 64 bit windows that have WOW64 installed (a removable option with Win2k8 R2) and may not work at all on ia64 platforms!
It's really just so much simpler to provide separate installers that it's really just not worth it to bundle them. You'll be doubling or tripling the installer size, which may just turn off some customers. If it's an internal tool, then there's really no downside - having the raw msi available allows so many more (remote) installing options.
So in short: yes, you can, but not with an MSI.