There is so much going on musically in this song having to do with the guitar parts and their rhythms. In the verse, the main guitar melody counterpointing the vocal is so simple and unassuming that you maybe won't realize it will become one of your favorite music cues. During the singing, bouncing on top of that reggae beat, the guitars staccato tap little melodies that so craftily end ahead of the beat and carry out over. It creates an otherworldly feel that made me slightly uneasy at first hearing, like jazz but more mysterious.
The chorus guitar part again pulls this ahead-of-the-beat trick and combines it with minor chords that don't resolve as much as just hold until their sustain is gone. Bob Marley was so good at odd chord changes that at first don't feel like they're going to fit into the song and then find some almost overdue way of resolving back down into what's going on. Credit the rhythm section for really holding solid to what they're doing, keeping the backbone of the song strong.
Bob Marley's singing throughout is just outstanding, just pure love. He was so, so gifted, simply born with either a spotlight or a halo on him, maybe one in the same. And the backing singers go just as far to put everything in the mood.
Fun fact: The official music video for the song includes a first appearance by then-7-year-old Naomi Campbell.