Hawkeye1489: The "Fallout 4 GOTY" edition requires around 33 GB and "Fallout London" around 34 GB of storage space... so that's about the 64 GB you mentioned.
Undead_Lilith: I should have clarified, the FO4 and FO London folders are separate, I was expecting each to be around 30GB (as advertised on the GoG website), but the FO4 file doubled in size to 64 GB... so now both files together are over 90GB. That is my problem =(
Then the "FO4" folder probably contains the complete installation data (as it should)... in this case you have the "London" installation twice on your hard drive.
Look in the "data" folder of the original "FO4" installation... to see if, for example, the same "LondonWorldSpace" files are in there as in your other folder.
"London" must be installed in the folder where the data for the original game is located.
Two separate installations of "Fallout 4", one for the unmodified original game and one for "London", do not work (unless you have it on Steam and then again on GOG and those two versions are installed to separate locations; in that case, both versions will access the same INI files and that will definitely cause problems).
That is why there is a note on the shop page that "London" makes irreparable changes to the original installation.
That's not entirely true, because it is possible to use the original and the mod in parallel. However, it is quite complicated to set up.