Clone Wars to break the Jedi, and he was successful. As the conflict escalated, the Jedi became increasingly cut off from the Force, overwhelmed by the fear and violence around them. Palpatine's scheme built to a climax with Order 66, which turned the Grand Army of the Republic against its Jedi Generals.
Order 66 was not a one-time event, however; rather, when Palpatine invoked it, it became law. From that moment on, Jedi were hunted across the galaxy; Darth Vader was placed in command of a group known as the Inquisitors, Force-s who had the power and authority to slaughter any Jedi they encountered. The true horror of the Inquisitors can be seen in the Obi-Wan Kenobi Disney+ TV show, when Obi-Wan breaks into their base - the Fortress Inquisitorius - and discovers a sickening trophy room, where the bodies of fallen Jedi and other Force-sensitives are kept. Darth Vader and his Inquisitors became Palpatine's enforcers, the hunters who would ensure the light of the Jedi never shone again.
Crimson Reign #3, by Charles Soule and Steven Cummings, reveals Order 66 was actually changed several times. In one flashback scene, a former lecturer at the University of Bar'leth - a specialist in the dark side of the Force - is harassed by a group of Imperial Stormtroopers. They invoke Order 66 Codicil Nine, which apparently brands some artifacts "illegal contraband." A codicil is a legal amendment, and the reference to "Codicil Nine" means there must have been at least another eight amendments. The original Order 66 was targeted against the Jedi alone, but Palpatine clearly extended it.
What Did Order 66 Come To Mean?
The Emperor didn't just want to destroy the Jedi; he also wanted to secure his Empire against any other threats, meaning other Force cults would have been branded illegal as well. It's interesting to note that, to date, the Guardians of the Whills are the only Force cult known to have operated in the open during the Dark Times of the Empire's rule. Although they venerated the Force, the Guardians of the Whills do not appear to have been Force-sensitive themselves, which was presumably what allowed them to continue existing. It seems the Emperor further established codicils requiring any and all artifacts to be seized by the Empire; he was always interested in acquiring dark side artifacts, so he'd have taken great pleasure in collecting them.
The most sinister aspect of Order 66 probably lies in the Inquisitor's most disturbing task; to scour the galaxy kidnapping children who possess the Force. The Emperor sought to acquire such children as part of what he called "Project Harvester," where children were turned to the dark side and used as a lens to help the Emperor watch his enemies and plan for potential threats. Nobody was likely to challenge the legal right of Darth Vader and his Inquisitors to take these children; but a codicil of Order 66 likely provided a basis for it all the same. Most Star Wars fans have assumed Order 66 was a singular event put in motion by Emperor Palpatine, but in reality it seems it was a law, one that became even more restrictive and horrific as the decades ed.