My apologies for the tech slang, but as I failed to explain with the sort version, here is the extended one:
LargeAddressAware is a flag that may or may not exist in all windows exe (and other) files. The tool you linked just make that, set the flag on the exe.
But I didn't used the tool; I used dumpbin.exe, that is a Microsoft tool that come with Microsoft Visual Studio and I am sure you can use more tools to check it (cff explorer for example is another tool that shows you that flag). And what I did was to check TS3W.EXE and guess what? My TS3W.EXE have already the LargeAddressAware flag set.
Now it may be possible that different versions of that file exist. You can see what version is your own file by right clicking the file and selecting properties, then in the details tab you will see a product and file version. The TS3W.EXE file I checked and that have already the LargeAddressAware flag is version 0.2.0.188.
So is a fact that EA maybe in the past delivered 32bits executables that cannot handle more than 2GB (indeed, 2^31 bits), but the one I have, delivered by EA on January 30 2013, can properly handle an address space of 2^32-1 bits. So i don't need to patch it with the tool that you linked.
Now we can also talk about that sims3.ini file and the non sense 8 digits value of MemoryUsageLimit. What represent 2.0e+7? twenty millions of what? They are not bytes for sure, there are 2.14e+9 bytes in a GB. They aren't Kb also, as there are 2.09e+6 KB in two GB. Maybe is heximal notation, then we are looking for something like 536 millions of something. Hmmm now that I look at it, the gpu reserves around 500Mb for TS3W.EXE... maybe it refers to graphic memory usage.