After Walt's realisation that Gus Fring needed to die in order for him to survive, he knew he needed to win Jesse back onto his side. Since his partner had been growing closer to the boss, seemingly being picked as the cook to move the project forward, Walt had to drive something between the two. He needed Jesse to want Gus dead just as much as he did.
Pinkman had always had a way of connecting with children, and this was no different with his girlfriend Andrea's son, Brock. Walt saw this as his opportunity, and used it to do what he did best, manipulating his naive partner. Using the Lily of the Valley from his back garden, Walt was able to poison and hospitalize Brock.
Since Jesse had already been at odds with Gus previously over the use of children in his business, in the chaos surrounding the boy's mysterious illness, Walt had little trouble convincing Jesse that this was the work of Fring, trying to turn them against each other.
Of all the horrible, heinous, unspeakable things Walter White did since his 50th birthday, risking a small, innocent child's life without a moment's hesitation just to stop Jesse from growing closer to Gus is the absolute worst.
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