Addendum: You could (re-)compress the uncompressed .cue and .bin pairs (or multiples) to the CHD format with will often shrink them up to around 50% of their former size and put them into just one file you can drop into your roms/psx directory. In my experience, those CHDs will run in 80-90% of the cases.
This one-liner will do that with all cue files and their corresponding bin files in the current directory.
for i in *.cue; do chdman createcd -i "$i" -o "${i%%.*}.chd"; done
Important: This will cut off the filenames after the first dot for the output CHD filenames. Remove one % from "${i%%.*}.chd to cut only the last extension for compatibility with filenames with multiple dots.
Beware though that this will only work with single-disk games. For storing multiple disks in one container you'll need the PBP format, which is also supported by Retropie's PSX emulators.
That said, be sure to check https://retropie.org.uk/docs/Playstation-1/ to see which emulators support CHD if you want to go that road.