Thank you!
The write speed of the rMBP SSD is around 7-800MB/s, I can't seem to find the speed of the 128GB SSD of the Fusion drive anywhere :/
Splitting the Fusion drive, will that make a noticeable difference?
I use my iMac for high end Retouching, Photography and Design, and also a bit of 4K video/timelapse editing – would I benefit more with just adding the 512GB SSD as an external scratch disk instead maybe?
I have a 2017 iMac too (5K model) but with the 1TB Fusion and wanted to do the same, since I didn't realize that the 1TB Fusion is only a 24 or 32GB SSD. Short answer is just sell the SSD and use the iMac as is (or upgrade the internal SSD).
I tried a Samsung 2.5" 512GB SSD in a USB 3.1 Gen 2 enclosure with proper USB-C cable and while it was generally fine, there were hiccups, times when the system would freeze for a few seconds, etc. It wasn't really that good as the main drive. I then bought a 512GB SSD to install, but didn't realize the new 2017 iMacs (at least the 5K version) use a completely different NVMe SSD (SSPOLARIS). The previous generation SSDs from 2015-16 (SSUBX) do fit, but don't boot - trust me I tried.
These new NVMe drives in your iMac are extremely fast, and from what I understand are basically Samsung 960 Pro drives (~3500MB/s read, ~2100MB/s write). I ended up replacing the 1TB HDD with the Samsung 2.5" SSD, and created a Fusion drive out of the small Apple SSD and the Samsung 2.5" one.
Therefore, your 2TB Fusion has an extremely fast 128GB NVMe SSD, and I think you should try it first since 128GB is actually fine for most people. I don't even think there is an enclosure for your Apple SSD from the MacBook. In any case, you won't like booting from a USB drive, even USB 3.1 Gen 2. If you really want more SSD space, I'd ideally buy an Apple NVMe SSD from eBay (make sure the label says SSPOLARIS) and an install kit from iFixit and just upgrade what you have. If you want to save some money, you can also replace the HDD with a regular 2.5" SSD.
Feel free to reach out if you want more help.