It depends on the severity of the paint defects you're trying to remove/correct.
I would suggest going with #80 first, then step up to #83 only if #80 isn't abrasive enough to correct what you're working on. If you use #83, you may need to finish off with #80.
Start off with the least abrasive polish first, then move on to something stronger if needed. You can do the same theory with your pads, before switching to a stronger (more abrasive) polish you can try a step up in pads. After a little experience you will be able to judge the condition of the finish and what to start off with easier. Until then it's best to play it safe.