According to most estimates, cows. While bison are estimated to produce about 72kg of methane per head per year, dairy cows are estimated to produce over 100 kg per head per year, and beef cows 76. When you further consider that there are significantly more cows than buffalo (there were an estimated 30,000,000 buffalo roaming the Great Plains back in the day, and in 2008 there were approximately 96,000,000 cows), the cows clearly come out on top.
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