A good, fast SD card is certainly a key point in getting good performance on RPi (and all other SBCs that use SD as storage). Random write speed is also important, especially if you use PVR which regularly updates the EPG database.
Personally I use Sandisk Extreme Pro 32GB micro SD cards and I'm quite satisfied with overall performance on RPi.
Another point is to stay away from "heavy" skins. The stock Estuary skin and eg Confluence are fine but others that use tons of effects, lot of huge textures etc won't be fun on RPi - it's GPU isn't exactly high end.
If you already have the RPi I'd also recommend to just invest the ~10 bucks for a good SD card, make sure you have a quality HDMI cable (the official RPi one will be fine for 4kp60) and give it a try,
My recommendation would be to use the latest LE11 nightly build as it contains a couple of important fixes since the latest official LE11 release. Get it from here:
https://test.libreelec.tv/11.0/RPi/RPi4/
so long,
Hias