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GPO assigned application needed for x86 and x64?

How does this work?  I want to assign 7-zip via GPO to my domain machines.  I have a mix a 32  and 64 bit machines in the PC OU.  Can I create 1 GPO and assign both apps in the GPO or do I have to assign a GPO for the 32bit version and 1 for the 64bit version of 7-zip?  
I assume I would have to add another OU (x86 and x64) under PC and move machines into the correct OU?  I would then link the correct GPO to the correct OU.

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Yes, you assume correctly. Two different OU would be needed for the respective packages
You dont need to move the computers to two seperate OUs. You will need to create two group policies and then link them to the same OU. You can use WMI filtering so that the package is only applied to the correct OS type.

You can use the Win32_Processor addresswidth attribute to determine 32bit and 64 bit os. This way only the 64 bit will get installed on 64 bit and 32 on 32 bit.