Seriously hurting, endangering, and even killing Padme earlier would have done this.
Consider this: at the beginning of the film, Padme believes she can negotiate a peaceful resolution to the Clone Wars (invent a reason this would be believable; I'm not trying to actually write this here) and wants to join the Republic forces. Anakin is afraid for her safety, but with Padme insistent, the Jedi Council allows Padme to come with them. Negotiations fail, lasers and explosions go off, and Padme is put into a terrible, critical condition (probably with a little help from Palpatine...)
With his heart dying, Anakin becomes colder and angry, internalizing all of his wrath and hurt, bringing him down to that dangerous, Darth Vader-style anger. The Jedi sense this roiling inner evil in Anakin and put him on Jedi probation. Of course, this only makes him worse, and Palpatine offers to help with the Dark Side.
Here, Anakin's tone shifts from petulance to dark anger (more in line with Vader) and his revenge on the Jedi is not just him trying to negotiate a happy ending for Padme. In ROTS as-written, Anakin betrays the Jedi in exchange for Palpatine's knowledge of how to save her life. When this didn't happen, you'd think Anakin would at least leave the Emperor's service, feeling betrayed, or possibly even kill him. I know Palpatine tells Anakin that Anakin killed Padme, but I feel like he'd figure out the truth. Over the years, this wouldn't turn him into the evil Lord of the Sith, it would make him sad and rethink his actions.
Of course, for this to work, it'd be better to have a subtler shift in Episode II as well. Off the top of my head, having Anakin defy the Jedi in ways that are almost "fun". Like, they say, "Don't rush in," and he goes in guns blazing and wins. Or they say, "Don't use all your power," and he pulls off a flawless victory with maximum force (or Force), maybe even with a bit of panache and a punchline. Anakin looks almost like a Han Solo type rascal, but he's learning that ignoring the Jedi and abusing his power are things that are not only effective, they're fun. As the film goes on, he could do this in darker ways (honestly, killing the sand people in revenge for his mom is a good way to show this, so... it's not like everything in the Prequels was bad). This would set up his hunger for power so that all ROTS would need to do is the shift into (a) commitment to the Dark Side, and (b) a shift of personality to Darth Vader's cold brutality.
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