As someone whose first RE completion was also RE4 (the PSX games were too scary for me as a kid), and holds RE4 as a top 3 favorite at least, I say you should definitely go for REmake next. It's still the pinnacle of the original RE style, and just an incredibly satisfying game. It'll give you context for the shift RE4 was for the series, and despite RE4 being very different in so many ways it still has a strong vein of resource management and some of the adventure style structure that the original games were founded on. That structure was completely ditched in 5 and 6 and only came back in a real way in 7, though even there it was somewhat watered down. If you enjoyed RE4 as an adventure, and not just a pure action rollercoaster, you'll find a ton to love in REmake.
You might want to emulate it rather than playing the HD Remaster, since that has odd choices like the ugly color grading, unfortunate losses in visual quality where some areas had to be redone as realtime environments because the original files were lost, and complete oversights like some music playing at double speed because of the higher framerate. Don't be afraid of tank controls, they work perfectly with the static camera and are really the only good solution to control with that style of camera. You get used to them pretty quickly. A tip for that: holding the interact button will cause you to go through any door you touch as soon as you touch it. It's a small but great piece of functionality that helps smooth out navigation further, because it lets you focus on steering your character. Just one reason that REmake is the most polished iteration of classic survival horror ever.
