The Brazilian Wandering Spider is at the top of most lists concerning this question.
What probably pushes this spider over the edge is the outright aggression it exhibits, and willingness to sink it's fangs into anything that is in its path.
The only other spider that might contest this is the Funnel Web Spider, with over 40 different toxic proteins in its venom. (The Funnel Web is also known for its aggressive behavior, with many accounts of the spider actually running after people!)
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