Turns out I was far from the only one who watched that show and felt like firing up Fallout 4 again, with mods of course 😄
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Other 196's:
There are 2 components, the background and the slides. I didn't touch most of the slides, because I realized they would need more than a simple upscale. The ones I did upscale I used waifu2x for. For everything else I used waifu2x, GIMP and Paint.NET.
waifu2x was an okay upscaler back in 2018. Today I would use StableSR or SUPIR.