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His choice of One Kind For Me was even more straightforward. If he was going to go all in, then why not go all in? If he focused his Beast Taming on snakes and serpent creatures alone, he would gain an intimate understanding of them and even gain their Beast Totem. Maybe, that Beast Totem would synergize well with his Madness and even accelerate his Comprehension speed.
Finally, there was Taboo Bond. It was the one that filled him with the most trepidation, but it was also because of this that he felt he had to choose it.
Setting aside how well it synergized with both other Paths, how it could allow him to both intimately understand the snake species and improve them… Sylas also had motives outside of this as well.