Captain Marvel
SHAZAM!
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In "Ultron Unlimited", which is arguably the best story written about the villain, Ultron massacres an entire European nation via drone assault (tanks and jets) and begins transforming the corpses into robot/zomie hybrids with the goal of creating a "master race" of hybrid organic/synthetic humans. Presumptively, Ultron would use the army to slowly destroy neighboring populations and convert them while spreading across the globe like a plague. This would probably be too dark for Disney though. (Although, this story does focus on Vision, the Scarlet Witch, and Pym).
In the first arc of Mighty Avengers (2007), Ultron attempts to kill the world's population through weather manipulation (natural disasters) created by hacking into Stark statellites meant to stabilize weather patterns. When this plan fails, Ultron begins hacking into nuke bases and launching missiles (ala Skynet in the Terminator series).
In the (terrible) Age of Ultron (2013), Ultron seemingly conquers the planet with an army of robots built in its likeness. How it built such a massive army is not explained.
In Annihilation: Conquest, he interfaced with the mechanical aliens called the Phalanx and took them over.